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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2024 , Vol. 36 >Issue 7: 975 - 986

DOI: https://doi.org/10.7536/PC231203

Review

Piezoelectric Biosensor and Its Application in Healthcare

  • Xingping Zhong 1 ,
  • Yanxia Chen , 1, 2, * ,
  • Chen Chen 1 ,
  • Lei Qin 1 ,
  • Xueji Zhang 3
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  • 1 Beijing Key Laboratory of Sensors, Beijing Information Science & Technology University, Beijing 100101, China
  • 2 School of Medicine, Tsinghua University, Beijing 100084, China
  • 3 School of Biomedical Engineering, Shenzhen University, Shenzhen 518060, China
* e-mail:

Received date: 2023-12-14

  Revised date: 2024-04-09

  Online published: 2024-07-01

Supported by

National Natural Science Foundation of China(22004009)

National Natural Science Foundation of China(U2006218)

Beijing Natural Science Foundation(2214057)

R&D Program of Beijing Municipal Education Commission(KM202111232005)

Project of Construction and Support for high-level Innovative Teams of Beijing Municipal Institutions(BPHR20220124)

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Abstract

With the rapid development of social economy and the continuous improvement of people's living standards,medical and health care have taken on an important strategic position.as an important analytical detection method,biosensing technology plays a key role in the field of medical health.piezoelectric biosensor,as a new kind of biosensor,utilizes piezoelectric materials for biological analysis.piezoelectric biosensor has the advantages of good stability,fast detection speed,high accuracy and simple operation,and has important application value in biomedicine,health monitoring and disease prevention and control.Herein,we review the research progress of piezoelectric biosensor home and abroad in recent years,and introduce the principle of piezoelectric biosensors based on the piezoelectric effect of quartz crystal microbalance and the commonly used piezoelectric materials,including inorganic piezoelectric materials,organic piezoelectric materials,piezoelectric composite materials and biological piezoelectric materials.in addition,the applications of piezoelectric biosensors in human health monitoring and disease prevention and control are also introduced,such as the monitoring of physiological signs,such as heart rate,blood pressure and pulse,the detection of biomarkers and epidemic viruses such as SARS-CoV-2(COVID-19).Finally,the current problems faced by piezoelectric biosensors are summarized,and the future development of piezoelectric biosensors is prospected。

Contents

1 Introduction

2 Working principle

3 Piezoelectric materials

3.1 Inorganic piezoelectric materials

3.2 Organic piezoelectric materials

3.3 Piezoelectric composite materials

3.4 Bio-piezoelectric materials

4 Applications in healthcare

4.1 Monitoring of physiological indicators

4.2 Biomarkers detection

4.3 Epidemic disease prevention and control

5 Conclusion and outlook

Key words： biosensor; piezoelectric materials; biomarkers; disease prevention and control; piezoelectric effect

Cite this article

Xingping Zhong , Yanxia Chen , Chen Chen , Lei Qin , Xueji Zhang . Piezoelectric Biosensor and Its Application in Healthcare[J]. Progress in Chemistry, 2024 , 36(7) : 975 -986 . DOI: 10.7536/PC231203

1 Introduction

biosensor is an instrument that combines bioactive materials with physicochemical converters for analysis and detection.After several generations of development,the research of Biosensor has made rapid progress[1⇓⇓⇓⇓~6]。 with the addition of physics,chemistry,optics,thermology and other disciplines,biosensors With different principles have been developed and utilized one after another.as one of the branches of biosensors,piezoelectric biosensors have been born,which have the advantages of good stability,fast detection and high sensitivity,and have potential applications in many fields such As environment,medicine,food and so on[7][8,9][10]。
in recent years,the research of piezoelectric biosensors In the field of health care has gradually increased.Especially with the emergence of the COVID-19 epidemic,biosensors are placed on higher requirements,not only to be fast and accurate,but also to be easy to operate.the progress of piezoelectric biosensors provides new opportunities to meet the detection needs[11]。 in addition,with the introduction of new piezoelectric materials and the in-depth study of material properties,the rapid development of piezoelectric biosensors in the field of health care has been greatly promoted[12⇓~14]。 in this paper,the main working principle of piezoelectric biosensors and piezoelectric materials are introduced,and the applications of piezoelectric biosensors in human health monitoring and disease prevention and control are summarized.Finally,the future development of piezoelectric biosensor is prospected.It is hoped that this review will draw people's attention to piezoelectric biosensors,promote their development in the field of health care,and provide ideas for the research of new piezoelectric biosensors。

2 Principle of operation

piezoelectric biosensor consists of piezoelectric material and biometric system.Biosensing based on the piezoelectric effect of piezoelectric quartz crystal is the most widely used.It usually means that the oscillation frequency of the sensitive element changes due to the change of its surface quality[15,16]。 the equation for the relationship between the mass and frequency of a piezoelectric quartz crystal was first proposed by Sauerbrey in 1959:[17]
$ \Delta F=-K F^{2} \Delta M / A$
Where∆F is the change in oscillation frequency(in Hz)due to a change in the surface quality of the crystal;K is a constant;F is the fundamental oscillation frequency of the piezoelectric material itself(in MHz);∆M is the change in the surface quality of the crystal;A refers to the area covered by the adsorbed substance on the surface of the sensitive material。
quartz crystal microbalance(quartz crystal microbalance,QCM)biosensor is a biodetection technology developed based on the piezoelectric effect of quartz crystal.Its working principle is to modify and fix bioactive molecules(such as biological receptors,antibodies,DNA,enzymes or cells)on the surface of quartz crystal(Figure 1A),and the object to be detected changes the surface quality of the crystal by combining with the recognition element,thus causing the oscillation frequency to change(from high frequency to low frequency),so as to achieve sensitive detection of the object to be detected[18,19]。 Abdul et al.coupled gold nanoparticles to DNA to significantly increase the mass of the QCM surface and improve the sensitivity of detection(Fig.1b)[20]。
图1 压电生物传感器：（a）石英晶体微天平；（b）DNA压电生物传感器[20]

Fig. 1 Piezoelectric biosensor：（a）Quartz Crystal Microbalance; （b）DNA piezoelectric biosensor [20]. Copyright 2016, Elsevier

3 Piezoelectric material

the development and utilization of piezoelectric materials have greatly promoted The development of piezoelectric biosensing technology[21,22]。 piezoelectric materials include inorganic piezoelectric materials such as quartz crystal,lead zirconate titanate piezoelectric ceramic transducer(PZT),zinc oxide,etc.,organic piezoelectric materials,mainly polyvinylidene fluoride(PVDF),piezoelectric composites,and biological piezoelectric materials such as DNA film,DNA chain,and peptides,etc[23⇓~25][26][27][28,29][30,31][32][33]。 Table 1 summarizes the types and applications of piezoelectric materials。
表1 Types and Applications of Piezoelectric Materials

Table 1 Summary of types and applications of piezoelectric materials。

Type Materials Applications Ref
Inorganic Quartz crystal Bilirubin, Bacteria, Uric acid 34,36,37
PZT Self-powered, Joint, Virus 40,41,42
Zinc oxide Swimming, Fingerprint 46,47
Aluminium nitride Escherichia coli, Sweat 49,50
Barium titanate Glucose 51
Organic Polyvinylidene fluoride Microdeformation, Body signs, bacteriostatic 53,54,56
Polyhydroxybutyrate Bio-scaffolds 57
Polyvinylidene-fluoride-trifluoroethylene Bacteriostatic 57
Composite Piezoelectric 1-3 composite material Blood pressure 60
Glycine - chitosan composite material Biomedical 61
Gold modified barium titanate Bacteriostatic 62
Biologic Diphenylalanine film Biosensing 65
γ -glycine crystal Biosensing 66
Across a membrane proteincrystal Tissue regeneration 67
DNA membrane Biological 69

3.1 Inorganic piezoelectric material

3.1.1 Quartz crystal

in 1880,the Curie brothers discovered the Piezoelectric effect on quartz crystal,which laid the foundation for the study of piezoelectric sensors.piezoelectric effect is a phenomenon In which a crystal is subjected to external mechanical pressure and charges are generated on its surface[34]。 Quartz crystal is divided into natural crystal and artificial crystal.It is a piezoelectric material with high mechanical strength and good temperature stability.It can maintain its piezoelectric characteristics even up to the Curie point temperature(575℃)[35]。
Wang et al.Used a quartz crystal microbalance to detect Campylobacter jejuni[36]。 Sensitive detection of Campylobacter jejuni was achieved by amplifying the QCM signal with antibody-coated gold nanoparticles.Zhang et al.Prepared red mud/molecularly imprinted polypyrrole particles by molecular imprinting technology,and modified them on the QCM electrode by surface modification to achieve specific recognition of bilirubin[34]。 The piezoelectric biosensor can be repeatedly used and can be stored for a long time.In addition,the molecularly imprinted TiO2was immobilized on the QCM electrode to detect uric acid,and the sensor showed a good linear relationship in the range of 0.04~45μmol/L[37]。 Zhou et al.Developed double resonator piezoelectric cytometry(DRPC)based on QCM to realize the simultaneous quantitative measurement of cell force and viscoelasticity[38]。 Based on the new technology of DRPC,the mechanical properties of cells can be monitored in real time and non-invasively,so as to distinguish apoptosis from apoptosis of HeLa cells,which provides a new method for cell death detection and drug evaluation[39]。

3.1.2 Lead zirconate titanate piezoelectric ceramics

PZT has the advantages of high mechanical coupling coefficient,high Curie temperature and good temperature characteristics.Different PZT-type piezoelectric ceramics can be constructed by adding element modification or replacing lead element with other elements,which greatly expands the application range of piezoelectric ceramics[21]。
PZT is commonly used to make self-powered devices and piezoelectric cantilever sensing devices.PZT continues to develop in the direction of flexibility,such as using PZT to make wearable devices to monitor human movement.Park et al.Fabricated a flexible PZT thin film nanogenerator[40]。 A PZT film with a thickness of 2µm was deposited on a sapphire substrate by sol-gel method,annealed and transferred to a plastic substrate coated with UV-sensitive polyurethane,and then irradiated by a laser to separate the PZT film from the substrate.the piezoelectric properties of the PZT film prepared in this way were greatly improved,and the PZT film still maintained a stable output voltage after 9000 times of bending.When the human body moves irregularly and slightly,the PZT thin film nanogenerator has a high-energy current signal output,which can control multiple LED arrays without external power supply at the same time,providing a new idea for the development of self-powered medical devices(Figure 2a)。
图2 无机压电材料：（a）PZT薄膜[40] ；（b）PZT薄膜压电生物传感器[41] ；（c）ZnO纳米线自供电生物传感器[46]

Fig. 2 Inorganic piezoelectric materials：（a）PZT thin film [40]. Copyright 2014, Advanced Materials（b）PZT thin film piezoelectric biosensor[41]. Copyright 2022, IEEE（c）Synthesis of self-powered biosensors based on ZnO nanowires [46]. Copyright 2021, Biosensors

Yeh et al.Fixed PZT as a sensitive material on a silicone plate,and then integrated it on a kinematic tape through an adhesive.the piezoelectric biosensor can be attached to the joint to detect the movement of the human body[41]。 At the same time,small holes are attached to the patch,which can detect perspiration during exercise through capacitance changes(Figure 2B).Lin et al.Designed a wearable ultrasonic patch system based on piezoelectric sensitive material PZT-5H,which integrates the ultrasonic probe and control electronics into a flexible wearable device to achieve long-term autonomous detection of central blood pressure,heart rate and cardiac output,and improves the accuracy of its detection through machine learning algorithms[42]。 PZT piezoelectric materials can also be Used to design cantilever structures.Katta et al.used metal platinum as an electrode and silicon as a substrate to sandwich the sensitive material PZT-5H to form a cantilever structure.One end was fixed on the substrate for integration with electronic circuits,and the other end was designed with a small groove for molecular adhesion,so that the antigen could be combined with the antibody[43]。 According to the specific adsorption of different kinds of antigens to detect a variety of tropical diseases,the specific detection of diseases can be realized from a variety of virus/parasite mixed samples,and the error is low,the accuracy is high,and the response is good.However,how to solve the problems of toxicity and flexibility of PZT sensors needs further study.Huang et al.Enhanced ductility and reduced toxicity by mixing a polymer hydrogenated styrene-butadiene block copolymer with PZT and encapsulating it in the polymer[44]。 the treated PZT piezoelectric biosensor has good flexibility and low toxicity,and can realize The detection of various physiological indexes。

3.1.3 Zinc oxide

As a green energy piezoelectric material,the preparation of zinc oxide is simple,and the zinc oxide can be used for manufacturing a piezoelectric nanogenerator with high power generation efficiency and fast response speed[45]。 Mao et al.Used zinc oxide nanowire array to convert The energy generated by human movement into electric energy to monitor the swimming process in real time.different swimming postures will produce Different voltage output signals,which can monitor the movement specifications of athletes.the sensor has good waterproof performance(Fig.2C)[46]。 Bouvet et al.Used piezoelectric zinc oxide nanowires for fingerprint detection.When the sensor array is subjected to mechanical deformation,the ZnO nanoparticles generate a piezoelectric potential,which is read and collected by a circuit to reconstruct the 3D deformation field corresponding to the fingerprint[47]。

3.1.4 Aluminum nitride

the piezoelectric film prepared by aluminum nitride has good flexibility and chemical stability,is a high-quality piezoelectric sensing material,and can be used for The detection of microbial and human indicators[48]。 Fathy et al.Used aluminum nitride film for detection of Escherichia coli[49]。 A V-shaped microcantilever structure based on the gap method was fabricated,and E.coli was enriched in the gap between the fixed arm and the vibrating arm by electrophoresis to obtain higher detection sensitivity.At the same time,the surface of the aluminum nitride film is covered with a pH response hydrogel,and the hydrogel shrinks or expands by adsorbing sweat,so that the oscillation frequency of the aluminum nitride film is changed,and the pH in the sweat is detected[50]。

3.1.5 Barium titanate

barium titanate is one of the most important materials for piezoelectric biosensors because of its good biocompatibility.Selvarajan et al.Fabricated a glucose piezoelectric biosensor based on Barium titanate nanoparticles[51]。 glucose is oxidized on the barium titanate film to release electrons,which inhibits the formation of a positive piezoelectric voltage at one end and causes the output voltage to decrease,and the detection of glucose is realized by establishing a relationship curve between the voltage decrease value and the glucose concentration.In addition,barium titanate nanoparticles are also a dental filling material,and the piezoelectric properties of barium titanate nanoparticles make them highly antibacterial and mineralizing.Montoya et al.Added barium titanate piezoelectric nanoparticles to dental resin,which can effectively inhibit the growth of oral biofilm by 90%and avoid the production of enzymes and acid corrosion of repair materials[52]。

3.2 Organic piezoelectric material

organic piezoelectric materials are a special kind of organic molecules,which can deform and generate charges under the action of an electric field,and can also be excited by charges.Most organic piezoelectric materials,such as polyvinylidene fluoride and polyhydroxybutyrate(PHB),have the characteristics of good flexibility,wide frequency response range,strong corrosion resistance and easy processing into piezoelectric films。
the self-powered device made of PVDF can realize the accurate monitoring of human body signs.Zou et al.designed a flexible self-arching biosensor based on PVDF,which is composed of double-layer polydi methylsiloxane(PDMS),single-layer PVDF and Ecoflex.the different mass ratio of PDMS and Ecoflex makes the stress mismatch between the two materials,thus regulating the self-arching structure.the embedding of PVDF forms a nano-generator,which improves the signal-to-noise ratio and stability of the biosensor[53]。 the sensor can measure the waveform of the radial artery and effectively convert the mechanical signal into an electrical signal(Figure 3A).Ghosal et al.Used biological bacterial proteins to modify the microstructure of poly(vinylidene fluoride)to construct bio-organic membranes with porous structure[54]。 Compared with pure PVDF,the melting point and dielectric constant of PVDF mixed with protein are increased,and the piezoelectric voltage coefficient is doubled due to the porous structure and interface polarization effect caused by the addition of bacterial protein.the sensor can detect mechanical signals from different parts of the human body,such as wrist,throat,neck vibration,etc.the sensor can also detect the vibration of the vocal cords synchronized with the spoken words and generate electrical signals,which will be a boon for deaf-mute patients(Figure 3B).Inspired by biological tendons,Kim et al.Designed a PVDF piezoelectric biosensor,which can convert the mechanical signals generated by human stretching into electrical signals to monitor the movement of the upper body in real time[55]。 the sensor is light In weight,easy to wear,and less affected by human motion.in addition,most organic piezoelectric materials also show good antibacterial properties.The effects of PVDF on The growth of gram-positive staphylococci and gram-negative Escherichia coli were different under different piezoelectric stimuli[56]。 Based on the different resonant frequencies,the growth of gram-positive staphylococci was inhibited and promoted by PVDF,while the growth of gram-negative Escherichia coli was not affected,which pointed out a direction for the use of piezoelectric stimulation to control bacterial growth.Vatlin et al.Found that sonicated piezoelectric polyhydroxybutyrate(Figure 3C),polyvinylidene fluoride,polyvinylidene fluoride trifluoroethylene,and non-piezoelectric polycaprolactone polymer films could inhibit bacterial growth[57]。 Zhu et al.prepared a shape-adaptive fiber electronic skin(Fig.3D)with coaxial core-shell structure piezoelectric fiber as the sensing layer,flexible conductive fabric as the electrode layer,and high elastic polyurethane film as the substrate layer,which has broad application prospects in sports medicine,human-computer interaction systems,intelligent robots,intelligent prosthetics,and other fields[58]。
图3 有机压电材料：（a）基于有机压电材料PVDF的压电传感器[53]；（b）PVDF链与肽键结合[54]；（c）聚羟基丁酸脂压电材料[57]；（d）压电纳米纤维[58]

Fig. 3 Organic piezoelectric materials：（a）piezoelectric sensor based on organic piezoelectric material PVDF [53], Copyright 2020, Elsevier; （b）binding of PVDF chain to peptide bond [54], Copyright 2022, Elsevier; （c）polyhydroxybutyrate piezoelectric material [57], Copyright 2020, Polymers;（d）piezoelectric nanofibers [58], Copyright 2020, Elsevier

3.3 Piezoelectric composite

piezoelectric composite materials have high piezoelectric response and electromechanical coupling coefficient,and have higher thermal stability and mechanical properties than single piezoelectric materials[59]。 At present,there are many studies based on piezoelectric composites,and they have been applied in physical monitoring,medical diagnosis and antibacterial.For example,the 1-3 piezoelectric composite material is made into a flexible ultrasonic blood pressure sensor,the piezoelectric ceramic is used as a substrate,the sensing array is made by filling PDMS,and the stretchable sensing electrode is made based on silver nanowires,which solves the problem that the traditional rigid substrate does not match the human skin surface[60]。 By sending ultrasonic signals and receiving echoes,the conversion from the diameter of human blood vessels to the blood pressure waveform is realized,which makes up for the shortcomings of sphygmomanometer,arterial catheterization and photoplethysmography,such as large volume,invasiveness and narrow application area(Figure 4A)。
图4 压电复合材料：（a）1-3型压电复合材料[60] ；（b）甘氨酸/壳聚糖（glycine/chitosan，Gly/CS）膜压电复合材料[61] ；（c）金纳米粒子修饰钛酸钡纳米立方体（Au@BTO）压电复合材料[62]

Fig. 4 Piezoelectric composite materials：（a）1-3 composite piezoelectric materials [60]. Copyright 2020, IEEE; （b）Glycine/chitosan（Gly/CS）membrane piezoelectric composite material [61]. Copyright 2020, ACS; （c）Gold nanoparticles modified barium titanate nanocube（Au@BTO）piezoelectric composite material [62], Copyright 2021, Elsevier

Hosseini et al.fabricated a degradable flexible piezoelectric biosensor using glycine and water-based chitosan,which has potential applications in wearable biomedical diagnosis(Fig.4B)[61]。 Wu et al.Used gold nanoparticles to modify barium titanate to form a piezoelectric composite for sonodynamic therapy.After ultrasonic stimulation,the material showed good antibacterial effect on Gram bacteria(Fig.4C)[62]。 Chernozem et al.Used calcium carbonate（CaCO3）and PHB to construct piezoelectric composite scaffolds,which have remarkable effects in bone repair,tissue regeneration,drug delivery and antibacterial,and the loading efficiency of alkaline phosphatase and vancomycin is increased by 3.5 times and 4.6 times respectively compared with the original framework,which is a very promising piezoelectric composite[63]。 Takeda et al.Prepared barium titanate（BaTiO3）/PVDF composite and applied it to piezoelectric biosensor,which overcomes the disadvantages of large volume and high price of traditional quartz biosensor,and can detect infectious diseases with low cost,sensitivity and rapidity[64]。

3.4 Biological piezoelectric material

piezoelectric materials have been developed into a series of biological piezoelectric materials,such as diphenylalanine membrane,transmembrane protein and so on.the research and application of these biological piezoelectric materials have promoted The development of piezoelectric biosensors。
good biocompatibility is the inherent advantage of biopiezoelectric materials,which makes them have a Good development prospect in implantable devices.Romanyuk et al.Proposed a new method for the preparation of piezoelectric diphenylalanine(FF)thin films[65]。 The transformation from amorphous phase to crystalline phase was achieved by solid phase crystallization.FF powder was dissolved in a stock solution of hexafluoroisopropanol,and FF thin films were Prepared by spin coating.the nucleation and growth of highly oriented piezoelectric active regions were triggered by controlling The environmental humidity and temperature.The FF film has a lateral piezoelectric response of about 30 pm/V,which can be used in implantable and wearable devices due to its natural biocompatibility and good piezoelectric properties(Figure 5A).Yang et al.prepared a piezoelectric biomaterial film based onγ-glycine crystals by evaporating The solvent in the glycine-polyvinyl alcohol solution.The film has strong mechanical flexibility,higher piezoelectric constant than most bio-organic films and good uniformity[66]。 This bio-piezoelectric material is non-toxic and hydrolyzable,widening the path for implantable device research and development(Figure 5B).Zhang et al.Preparedβ-glycine nanocrystalline films by synergistic nanoconfinement technique and in situ polarization(Figure 5D)[67]。 the membrane has good output performance,natural biocompatibility and biodegradability,which provides a strategy for The construction of high-performance large-size piezoelectric biosensor interface materials。
图5 生物压电材料：（a）二苯丙氨酸（FF）膜[65]；（b）甘氨酸-聚乙烯醇复合薄膜[66] ；（c）跨膜蛋白ba3细胞色素c氧化酶晶体结构[68]；（d）β-甘氨酸纳米晶膜[67]

Fig. 5 Bio-piezoelectric materials：（a）diphenylalanine （FF） membrane [65], Copyright 2022, Elsevier; （b）Glycine - polyvinyl alcohol composite film [66], Copyright 2021, IEEE;（c）crystal structure of the transmembrane protein ba3 cytochrome c oxidase [68], Copyright 2023, Advanced Functional Materials; （d）β-glycine nanocrystalline film [67], Copyright 2023, Springer Nature

With the in-depth study of biological piezoelectric materials,the piezoelectric properties of biological proteins and DNA have been gradually discovered.In 2021,piezoelectric properties of single crystals of the transmembrane protein ba3C ytochrome C oxidase were discovered,broadening the scope of current research on biological piezoelectric materials(Figure 5C )[68]。 Yang et al.Found that DNA film has piezoelectric properties,and proposed the piezoelectric equation of DNA film.the study shows that the elastic modulus of DNA film is proportional to the absolute value of piezoelectric coefficient and the packaging density[69]。

4 Application in medical and health field

with The continuous development and utilization of piezoelectric materials,piezoelectric biosensors have been widely used in the field of health care.the accuracy and stability of sensing equipment are constantly improving,and it can also be combined With algorithms to detect heart rate,pulse pressure and other signals[70⇓⇓⇓~74]。 Compared with traditional optical,mechanical and ultrasonic methods,piezoelectric biosensors are more sensitive to human monitoring and simpler to operate[75,76][77,78][79]。 The research progress of several new piezoelectric biosensors in physiological indicators monitoring(heart rate,blood pressure,pulse),biomarker detection and disease prevention and control is introduced below。

4.1 Physiological index monitoring

heart rate,pulse and blood pressure are important physiological indicators of human body,which are closely related to human health and life safety.abnormal heart rate may be a potential manifestation of some heart diseases,while Abnormal pulse and blood pressure are usually associated with cardiovascular and cerebrovascular diseases.Therefore,the detection of these physiological indicators is very necessary。

4.1.1 Heart rate

heart rate is an important index to measure The function of cardiovascular system.Regular heart rate monitoring is of great significance for preventing heart disease,optimizing exercise plan and maintaining physiological health.Hu et al.Developed a wearable cardiac ultrasound imager,which selected 1-3 composite materials to transmit and receive ultrasound,and obtained the best signal-to-noise ratio and spatial resolution by means of wide-beam composite images.It breaks through the shortcomings of traditional cardiac detection equipment,which is bulky and unable to monitor continuously.the equipment has extremely high sensitivity and will play an important role in real-time monitoring of intensive care and cardiovascular diseases(Figure 6a)[80]。 fetal heart rate signal monitoring is very important for evaluating the health of the fetus.Nassit et al.Compared the effects of sensors made of PVDF and PZT piezoelectric materials on Fetal heart rate detection[81]。 PVDF-based sensors are superior to PZT in terms of cost,mechanical properties,human applicability,and response speed.non-contact measurement can solve the problem of discomfort caused by sticking sensors to the surface of the human body.Chen et al.Designed a hollow microstructure self-powered pressure sensor(HM-SPS)for Non-contact monitoring of sleep and heart rate[82]。 According to the electrostatic effect,HM-SPS detects the heartbeat and breathing signals and transmits them to the mobile phone.A dynamic pressure sensitivity of 18.98 V·kPa-1and an operating range of 40 kPa can be achieved simultaneously using only commercial polymer films.Fang et al.Successfully achieved non-contact heart rate signal acquisition with piezoelectric sensors[83]。
图6 生理性指标监测：压电生物传感器对（a）心率[80] ；（b）血压 [84] ；（c）脉搏进行监测 [90]

Fig. 6 Psychological indexes monitoring：（a）heart rate [80], Copyright 2021, Nature; （b）blood pressure [84], Copyright 2021, IEEE;（c）pulse [90], Copyright 2021, Sensors

4.1.2 Blood pressure

blood pressure monitoring mainly uses sensors to monitor the Blood pressure waveform of radial artery or carotid artery,and establishes the relationship between the output waveform and the voltage signal for real-time health monitoring。
Li et al.Made a 10×10 pulse wave array sensor with PVDF membrane,and combined with deep learning algorithm to realize radial artery waveform monitoring(Fig.6B)[84]。 In addition,Yi et al.Clarified the algebraic relationship between human arterial pulse and blood pressure and the influence of human joint motion on pulse wave,eliminated motion artifacts,and established a wearable system that can realize continuous blood pressure monitoring with only a single piezoelectric sensor[85]。 Lokesh et al.Designed a non-invasive piezoelectric blood pressure sensor with a cantilever structure using PZT,and the simulation results showed extremely high sensitivity and flexibility[86]。 Wang et al.developed a blood pressure test system for radial artery signal measurement.The sensing part is composed of PVDF film,which improves The ability to resist electromagnetic field interference during detection.The whole system is easy to operate,with high sensitivity and wide pressure detection range[87]。 On the other hand,the combination of PVDF film and dual-gate thin film transistor is used to construct a self-driven blood pressure monitoring sensor for blood pressure monitoring,and the actual test results fully meet the standards of the American Medical Instrument Testing Association[88]。 Heart rate and pulse pressure can also be monitored quickly,accurately and continuously by using the pressure generated by the human carotid artery on the sensor[89]。

4.1.3 Pulse

pulse is also an important indicator of human health.Guo et al.Proposed a piezoelectric pulse sensor,which can convert the abnormal pulse waveform generated by abnormal heart rate into electrical signal output[90]。 The Moens-Korteweg equation was used for analysis,which improved the accuracy of the test results(Figure 6C).The biopiezoelectric energy harvester(BPEH)is a new type of pulse wave monitoring device.Kar et al.Made BPEH using natural piezoelectric material chicken feather fiber[91]。 the BPEH has high mechanical strength,and can quickly charge the capacitor by 2.0 V in 3 min under the action of the finger.the BPEH is fixed on the wrist,and the capacitor is charged by pulse vibration,which can monitor the health status of the tester in real time.BPEH also has good biocompatibility and environmental friendliness.Zhang et al.Designed a smart textile wristband pulse sensor by fixing PVDF piezoelectric film on flexible fabric,and improved the piezoelectric performance of PVDF through the combination of liquid phase separation and stretching polarization process[92]。 In addition to wrist pulse monitoring,fingertip pulse wave measurement is also one of the research directions of pulse detection.Meng et al.Developed a self-powered hemispherical fingertip pressure sensor,which can detect the periodic signal generated by the tiny pulse beating on the fingertip and realize personalized medical monitoring[93]。 the sensor has a sensitivity of 49.8 mV/Pa,a response time of less than 6 ms,and a service life of more than 4 months.Sun et al.Used silver-coated PVDF on both sides as a piezoelectric material to make a self-powered multifunctional bracelet,which combines triboelectricity with piezoelectric nanogenerator to stably monitor the pulse signal of the wearer during exercise without external power supply[94]。

4.2 Biomarker detection

the detection of biomarkers can achieve the prevention and early diagnosis of diseases.for example,malignant tumors are fatal to the human body.Pohanka modified the surface of QCM with tumor factor antibody,and the piezoelectric sensor solved the problem of time-consuming enzyme linked immunosorbent assay(ELISA)detection,providing support For emergency testing(Figure 7A)[95]。 Su et al.Developed a PZT piezoelectric biosensor for cancer marker detection[96]。 the sensing and control unit consists of two ceramic resonators connected in parallel,which improves the sensing performance and enables the detection of trace samples with a sensitivity of 0.25 ng/mL.Proteases play an important role in human health,and the occurrence of many diseases is closely related to protein abnormalities,such as inflammation,autoimmune diseases and so on.Xi et al.Developed a piezoelectric biosensor for thrombin detection using a one-step incubation method.Gold nanocages loaded with polyamide and DNA probes were immobilized on QCM for specific aptamer hybridization of thrombin,which reduced the detection limit to 7.7 pmol/L(Figure 7B)[97]。 In addition,for the diagnosis of glomalin,Pohanka et al.Added iron oxide nanoparticles on the basis of quartz crystal immobilized glomalin antibody,which reduced the detection limit of the sensor,and was simple to manufacture and operate,and could be stored for a long time[98]。 They also immobilized the antibody doped with nano-iron oxide particles on a quartz crystal microbalance to determine protein Glomalin with good sensitivity and low detection limit。
图7 生物标志物检测：（a）肿瘤坏死因子（TNFα）检 测[95]；（b）凝血酶（Thrombin）检测[97]

Fig. 7 Biomarkers detection：（a）tumor necrosis factor assay[95], Copyright 2018, Elsevier; （b）thrombin detection [97], Copyright 2021, American Chemical Society

Nascimento et al.Developed a QCM sensor for autoantibody determination and detection of systemic lupus erythematosus(systemic lupuseryth ematosus,SLE)[99]。 the detection performance of the sensor can meet the ELISA standard when tested on SLE patients.Alzheimer's disease is a common disease in the elderly,and tau protein is the main marker.Li et al.Fabricated a quartz crystal microbalance immunosensor to achieve micromolar tau protein determination[100]。 Han et al.Modified polypyrrole conductive polymer film on the electrode surface of piezoelectric sensor to detect inflammatory factors,and found that the content of lipopolysaccharide and histamine could cause different internal offset rates of the sensor,which is expected to promote the research of piezoelectric sensor in cytology and toxicology[101]。 as an important energy source and metabolic intermediate of cells,glucose content is closely related to human health.Dou et al.Reported a glucose detection device based on a hydrogel-coated quartz crystal balance,which formed a gel on the surface of QCM by ultraviolet pressure polymerization,and was able to sensitively detect trace glucose in saliva,with a detection limit as low as 3 mg/L,which was reduced to 1/30 compared with the sensor prepared by the traditional spin-coating method[102]。 Perez-Vielma et al.Used QCM piezoelectric biosensor to study the interaction between bioactive peptides(Val-Pro-Pro,VPP)and specific gene sequences,and because of the high sensitivity of QCM,the interaction between VPP and genes can be detected[103]。 It provides an effective verification method for using VPP to regulate the expression of disease-related genes.Wang et al.Fabricated a self-powered piezoelectric biosensor using zinc oxide(ZnO)nanowires[104]。 The enzyme-modified ZnO nanowires can actively output an electrical signal related to the creatinine concentration through the piezoelectric effect and the coupling effect of the enzymatic reaction,and can realize the real-time detection of the creatinine level of a human body without an external power supply,with a detection range of 10-5~10-1mmol/L and a sensitivity of 0.0229 V/mM 。

4.3 Epidemic Disease Prevention and Control

Although The COVID-19 epidemic has been effectively controlled,it still poses a threat to human health,and the detection of COVID-19 is still very necessary.Abdullah et al.integrated the sensor and micro electro mechanical systems(MEMS)into the mask,which can realize real-time virus monitoring only by wearing the mask,and can detect virus particles with a diameter of≥100 nm.the sensor also has potential applications in other microbial detection(Figure 8A)[105]。 Forinov Forinováet al.Constructed a QCM sensor with anti-fouling function on the surface by using terpolymer,which can accurately identify SARS-CoV-2 after simple treatment of the sample,with short detection time,low detection limit and 1.3×104PFU/mL[106]。 Piezoelectric biosensor based on cantilever structure has good selectivity for the detection of novel coronavirus.Kabir et al.Immobilized the antibody on the cantilever surface to detect COVID-19 in clinical samples without any pretreatment and labeling[107]。 The piezoelectric MEMS microcantilever biosensor designed by Niranjan et al.Can rapidly and continuously respond to SARS-CoV-2 virus with a mass sensitivity of 20 copies/mL[108]。
图8 流行疾病检测：（a）可穿戴压电生物传感器检测病毒颗粒[105]；（b）艾滋病病毒检测[109]；（c）基孔肯雅病毒检测[111]

Fig. 8 Epidemic disease detection：（a）wearable piezoelectric biosensor detection of virus particles [105], Copyright 2021, IEEE; （b）HIV detection [109], Copyright 2016, Elsevier; （c）CHIKV detection [111], Copyright 2023, Macromolecular Symposia

Not only the novel coronavirus,but also the detection of other viruses by piezoelectric biosensors is under way.Ly et al.Used QCM for HIV-1 antigen detection,and modified gold nanoparticles with streptavidin on the surface of QCM for signal enhancement to achieve sensitive detection of samples with a concentration of 1 ng/mL(Fig.8B)[109]。 Pirich et al.Covered a quartz crystal microbalance with a layer of bacterial cellulose nanofiber membrane,and the combination of the two materials improved the sensitivity of the piezoelectric sensor to dengue non-structural protein antibodies and reduced the detection limit[110]。 Niranjan et al.designed a cantilever piezoelectric biosensor(Fig.8C)to achieve label-free and sensitive detection of chikungunya virus[111]。 PZT-5A,which can maintain stable piezoelectric properties at extreme temperatures and different changing temperatures,is used as The piezoelectric material,and the voltage,stress and displacement of three materials(silicon,gold and PDMS)are simulated and compared,and PDMS is the best choice for the cantilever.the biosensor can be used in remote and resource-poor areas because it does not require laboratory facilities to store and process samples or professionals for diagnosis。
the development and application of piezoelectric biosensors will help to improve the level of detection technology in the field of health care and life science research,and is expected to make greater contributions to human health。

5 Conclusion and prospect

in this paper,the working principle of piezoelectric biosensors and piezoelectric materials are introduced,and the applications of piezoelectric biosensors in human health monitoring and disease prevention and control are summarized.These piezoelectric biosensors have good stability and sensitivity,and have great potential application value in the field of health care and precision medicine.However,there are still many challenges to achieve portable,home,intelligent,real-time detection and other functions:(1)At present,more research is concentrated in the laboratory stage,which can not be put into large-scale production.It is expected to accelerate the marketization of piezoelectric biosensors by combining the data collected by sensors with algorithms and integrating large data for statistical analysis to achieve intelligent detection.(2)Compared with paper-based and fabric-based biosensors,the cost of piezoelectric biosensors is still high,and some piezoelectric materials are toxic and less environmentally friendly.Therefore,the development of new piezoelectric materials with low cost and good biocompatibility by modification and introduction of nanomaterials can provide a new design strategy for piezoelectric biosensors.(3)How to maintain the stability and durability of self-powered piezoelectric biosensors is still a difficult problem to be overcome.the performance of self-powered piezoelectric biosensors is expected to be improved by mixing a variety of piezoelectric materials or constructing new structures.(4)the high-throughput detection technology of piezoelectric biosensor needs to be further developed.Combined with microarray design,new methods are explored to improve the detection throughput of biosensors and improve the detection efficiency and accuracy of target analytes.Through the efforts of many researchers,new piezoelectric materials continue to develop in the direction of flexible and wearable,which provides a new boost for the development of piezoelectric biosensors.It is believed that piezoelectric biosensors will provide more convenient services for our lives in the future。

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