高效医学传感钙钛矿材料研究进展

doi:10.3866/PKU.WHXB202211025

物理化学学报 >> 2023, Vol. 39 >> Issue (5): 2211025.doi: 10.3866/PKU.WHXB202211025

高效医学传感钙钛矿材料研究进展

杨帅¹, 徐瑜歆¹, 郝子坤¹, 秦胜建¹, 张润鹏¹, 韩钰¹, 杜利伟¹, 朱紫洢¹, 杜安宁¹, 陈欣³, 吴昊⁴, 乔冰冰⁵, 李坚⁶^,⁷, 王艺¹, 孙昺晨¹, 闫融融¹, 赵晋津²^,*()

¹ 石家庄铁道大学电气与电子工程学院, 低碳高效能量转换材料与器件研究所, 石家庄 050043
² 河北师范大学化学与材料科学学院, 河北省无机纳米材料重点实验室, 石家庄 050024
³ 邢台市人民医院, 河北邢台 054001
⁴ 解放军第九八四医院中西医结合科, 北京 100094
⁵ 邯郸邯钢医院肿瘤一科, 河北邯郸 056001
⁶ 河北医科大学第二医院神经内科, 石家庄 050000
⁷ 衡水市人民医院全科医学科, 河北衡水 053000

收稿日期:2022-11-16 录用日期:2022-12-22 发布日期:2022-12-30
通讯作者: 赵晋津 E-mail:jinjinzhao2012@163.com
基金资助:
国家自然科学基金(U213012);国家自然科学基金(11772207);河北省自然科学基金(F2020210016);河北省自然科学基金(E2022210097);河北省自然科学基金-京津冀基础研究合作专项项目(H2022205047);中央引导地方科技发展资金项目(216Z4302G);河北省创新能力提升计划项目(22567604H);河北省青年拔尖人才支持计划项目及河北省市场监管局科技计划项目(2023ZC03)

Recent Advances in High-Efficiency Perovskite for Medical Sensors

Shuai Yang¹, Yuxin Xu¹, Zikun Hao¹, Shengjian Qin¹, Runpeng Zhang¹, Yu Han¹, Liwei Du¹, Ziyi Zhu¹, Anning Du¹, Xin Chen³, Hao Wu⁴, Bingbing Qiao⁵, Jian Li⁶^,⁷, Yi Wang¹, Bingchen Sun¹, Rongrong Yan¹, Jinjin Zhao²^,*()

¹ School of Electrical and Electronic Engineering, Shijiazhuang Tiedao University, Institute of Materials for Energy Conversion, Shijiazhuang 050043, China
² Hebei Key Laboratory of Inorganic Nano-materials, College of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, China
³ Xingtai People's Hospital, Xingtai 054001, Hebei Province, China
⁴ The 984th Hospital of the PLA, Integrated TCM & Western Medicine Department, Beijing 100094, China
⁵ First Medical Oncology, Handan Han Gang Hospital, Handan 056001, Hebei Province, China
⁶ Department of Neurology, The Second Hospital of Hebei Medical University, Shijiazhuang 050000, China
⁷ General Practice Department, Hengshui People's Hospital, Hengshui 053000, Hebei Province, China

Received:2022-11-16 Accepted:2022-12-22 Published:2022-12-30
Contact: Jinjin Zhao E-mail:jinjinzhao2012@163.com
Supported by:
the National Natural Science Foundation of China(U213012);the National Natural Science Foundation of China(11772207);the Natural Science Foundation of Hebei Province(F2020210016);the Natural Science Foundation of Hebei Province(E2022210097);the Natural Science Foundation of Hebei (The Basic Research Cooperation Special Foundation of Beijing-Tianjin-Hebei Region)(H2022205047);the Central Government Guiding Local Science and Technology Development Project(216Z4302G);the Innovation Capability Improvement Plan Project of Hebei Province(22567604H);the Youth Top-notch Talents Supporting Plan of Hebei Province, and the Hebei Administration for Market Supervision Science and Technology Project List(2023ZC03)

摘要/Abstract

摘要：

卤化物钙钛矿材料作为一种新型半导体材料，具有优异的光电转换特性、能级结构可调、易于加工、结构和尺寸以及形貌可调、改性后优异的生物相容性等优点，在医学检测传感器中具有广阔的应用前景。本综述讨论了钙钛矿材料在生物医学传感领域的研究进展，钙钛矿医学传感器能通过光电转换、全光转换、电催化等多种物理或化学机制实现传感，具有可灵活选择的器件结构、性能指标和信号传递方式，用于人体代谢物质、神经递质、癌症相关物质和药物等医学物质的检测。钙钛矿医学传感器将为未来的医工多学科融合提供新希望，加快医工融合发展。

关键词: 卤化物钙钛矿, 医学传感器, 光电转换, 全光转换, 电催化

Abstract:

Perovskite materials have considerable potential in medical sensors. This is because the diverse element substitution of the perovskite ABX₃ composition brings rich physical and chemical properties for perovskite materials, including photoelectric conversion, all-optical conversion, and electro-optical conversion. By modifying the A-site, B-site, or X-site elements, the bandgap width of perovskite materials can be adjusted. Moreover, the absorption spectrum, photoelectric conversion electrical signal, and all-optical conversion luminescence spectrum can be regulated in perovskite materials. Perovskite materials also have the advantages of easy fabrication, excellent biocompatibility after modification, variable chemical valence states of constituent elements, and adjustable morphology. Therefore, perovskite materials are expected to be used in medical sensors with different operation mechanisms, such as photoelectric sensors, all-optical conversion sensors, electrocatalytic sensors, physicochemically loading sensors, and surface plasmon resonance (SPR) sensors. Based on the photoelectric conversion mechanism, perovskite medical sensors can detect metabolic substances, cancer-related substances and drugs in three ways: hindering charge transfer, trapping charges, and changing the number of photo-induced carriers. Furthermore, perovskite photoelectric medical sensors exhibit an ultrasensitive detection performance, even reaching 10⁻³ fmol·L⁻¹. Based on the all-optical conversion mechanism, metabolite substances and drugs are detected by perovskite all-optical conversion medical sensors via electron/hole transfer, perovskite material degradation, or perovskite material phase transition. Perovskite all-optical conversion medical sensors can be used to detect medical substances based on precise measurement using the photoluminescence spectrum and direct estimation based on the visible color changes. Based on the variable chemical valence states of constituent elements for perovskite materials, metabolite substances, neurotransmitters, cancer-related substances, and drugs are detected by the perovskite electrocatalytic medical sensors via oxidation reaction or reductive reaction. These have variable electrochemical measurement methods for medical substances, such as cyclic voltammetry, amperometry, and differential pulse voltammetry. They can not only simultaneously detect multiple substances but also are biocompatible. Based on the physicochemical loading and SPR mechanisms, metabolite substances and cancer-related substances are detected. Perovskite physicochemically loading medical sensors can detect both liquid and gaseous substances by utilizing the electrical conductivity or adsorbability of perovskite materials, and the detection of perovskite SPR medical sensors will not damage medical substances. In conclusion, owing to the different operation mechanisms of perovskite medical sensors, they exhibit high sensitivity and precision for detecting a wide range of medical substances, which meets the diverse requirements of medical detection. Thus, perovskite medical sensors pave the way for future multidisciplinary integration and development between the medicine and engineering fields.

Key words: Halide perovskite, Medical sensor, Photoelectric conversion, All-optical conversion, Electrocatalysis

杨帅, 徐瑜歆, 郝子坤, 秦胜建, 张润鹏, 韩钰, 杜利伟, 朱紫洢, 杜安宁, 陈欣, 吴昊, 乔冰冰, 李坚, 王艺, 孙昺晨, 闫融融, 赵晋津. 高效医学传感钙钛矿材料研究进展[J]. 物理化学学报, 2023, 39(5), 2211025. doi: 10.3866/PKU.WHXB202211025

Shuai Yang, Yuxin Xu, Zikun Hao, Shengjian Qin, Runpeng Zhang, Yu Han, Liwei Du, Ziyi Zhu, Anning Du, Xin Chen, Hao Wu, Bingbing Qiao, Jian Li, Yi Wang, Bingchen Sun, Rongrong Yan, Jinjin Zhao. Recent Advances in High-Efficiency Perovskite for Medical Sensors[J]. Acta Phys. -Chim. Sin. 2023, 39(5), 2211025. doi: 10.3866/PKU.WHXB202211025

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202211025

https://www.whxb.pku.edu.cn/CN/Y2023/V39/I5/2211025

图/表 10

图1

图2

表1

图3

表2

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表3

钙钛矿电催化医学传感器的核心材料和器件性能"

Substance	Key materials	Detection range	Limit of detection	Sensitivity	Ref.
Glucose	NdNiO₃	0.5 μmol∙L⁻¹–4.6 mmol∙L⁻¹	0.3 µmol∙L⁻¹	1105.1 µA·L·mmol⁻¹·cm⁻²	68
	La_0.6Sr_0.4CoO_3−δ-reduced graphene oxide	2–335 μmol∙L⁻¹	0.063 μmol∙L⁻¹	330 μA·L·mmol⁻¹·cm⁻²	71
	LaTiO₃-Ag_0.1	0.01 μmol∙L⁻¹–0.10 mmol∙L⁻¹	2.50 nmol∙L⁻¹	780 μA·L·mmol⁻¹·cm⁻²	111
	LaNi_0.6Co_0.4O₃	0.05–200 μmol∙L⁻¹	8.0 nmol∙L⁻¹	643.0 μA·L·mmol⁻¹·cm⁻²	67
	LaTiO₃-Ag_0.2	2.5 μmol∙L⁻¹–4 mmol∙L⁻¹	0.21 μmol∙L⁻¹	784.14 mA·L·mmol⁻¹·cm⁻²	113
	LaCoO₃	10 nmol∙L⁻¹–407.2 μmol∙L⁻¹	1.6 nmol∙L⁻¹	3.279 μA·L·μmol⁻¹·cm⁻²	110
	Glucose oxidase/ SrTiO₃-chitosan	0.01–1.2 mmol∙L⁻¹	3 μmol∙L⁻¹.	15.6 mA·L·mol⁻¹·cm⁻²	112
	Sr₂Pd_0.7Au_0.3O₃	0.2–100 μmol∙L⁻¹	2.11 nmol∙L⁻¹	14.40 mA·L·mmol⁻¹·cm⁻²	107
	Glucose oxidase/ CaTiO₃-chitosan	7 μmol∙L⁻¹–1.49 mmol∙L⁻¹	2.3 μmol∙L⁻¹	14.10 ± 0.5 mA·L·mol⁻¹·cm⁻²	32
L-cysteine	LaNi_0.5Ti_0.5O₃	2.5–40 μmol∙L⁻¹	0.5 μmol∙L⁻¹	55 nA·L·μmol⁻¹	109
L-tryptophane		5–60 μmol∙L⁻¹	0.67 μmol∙L⁻¹	38.2 nA·L·μmol⁻¹	109
L-alanine		50–600 μmol∙L⁻¹	8 μmol∙L⁻¹	3.08 nA·L·μmol⁻¹	109
L-phenylalanine		25–500 μmol∙L⁻¹	3 μmol∙L⁻¹	3.84 nA·L·μmol⁻¹	109
Uric acid	SrPdO₃	-	-	-	69
Uric acid	FeTiO₃	1–150 μmol∙L⁻¹, 200–500 μmol∙L⁻¹	30 nmol∙L⁻¹	-	16
Urea	LaNi_xCo_1−xO₃	50 nmol∙L⁻¹–0.08 mmol∙L⁻¹	5.0 nmol∙L⁻¹	-	28
Dopamine	SrPdO₃	7–70 μmol∙L⁻¹	9.3 nmol∙L⁻¹	0.8807 μA·L·μmol⁻¹	69
	KTaO₃	0.5–4.5 μmol∙L⁻¹	-	-	70
	FeTiO₃	1–90 μmol∙L⁻¹, 110–350 μmol∙L⁻¹	1.3 nmol∙L⁻¹	1.56 μA·L·μmol⁻¹·cm⁻²	16
	GdTiO₃/graphene	72 nmol∙L⁻¹–1.5 μmol∙L⁻¹	96.89 nmol∙L⁻¹	3.357 ×10⁻⁵ A·L·nmol⁻¹	105
	LaMnO₃	1–600 μmol∙L⁻¹	32 nmol∙L⁻¹	1 µA·L·μmol⁻¹	22
	LaNi_xCo_1−xO₃	80 nmol∙L⁻¹–0.08 mmol∙L⁻¹	3 nmol∙L⁻¹	-	28
	LaBO₃ (B = Fe, Co, Ni)	80 nmol∙L⁻¹–20 μmol∙L⁻¹	9 nmol∙L⁻¹	-	117
L-dopa	SrPdO₃	0.6–9 μmol∙L⁻¹	1.63 nmol∙L⁻¹	0.7958 μA·L·μmol⁻¹	118
Serotonin	LaBO₃ (B = Fe, Co, Ni)	100 nmol∙L⁻¹–80 μmol∙L⁻¹	14 nmol∙L⁻¹	-	117
Tyrosine	LaBO₃ (B = Fe, Co, Ni)	0.5–70 μmol∙L⁻¹	56 nmol∙L⁻¹	-	117
Glutamate	NdNiO₃/Nafion/glutamate oxidase	1–700 μmol∙L⁻¹。	16 nmol∙L⁻¹	–	27
H₂O₂	BiFeO₃/Cress peroxidase	0.2–50 μmol∙L⁻¹	80 nmol∙L⁻¹	0.142 mA·L·μmol⁻¹·cm⁻²	108
	LaNi_0.6Co_0.4O₃	10 nmol∙L⁻¹–100 μmol∙L⁻¹	1.0 nmol∙L⁻¹	1812.84 μA·L·mmol⁻¹·cm⁻²	67
	La_0.6Sr_0.4CoO_3−δ-reduced graphene oxide	0.2–3350 μmol∙L⁻¹	0.05 μmol∙L⁻¹	500 μA·L·mmol⁻¹·cm⁻²	71
Atrazine	Al₂NiCoO₅	0.5 × 10⁻⁹–10⁻⁷ (volume fraction)	0.3 × 10⁻⁹ (volume fraction)	0.929 μA∙ppb⁻¹∙cm²	115
Amlodipine	NdFeO₃/glycine/carbon nanotubes	3 nmol∙L⁻¹–200 μmol∙L⁻¹	0.704 nmol∙L⁻¹	113.2 μA·L·μmol⁻¹	106
Ascorbic acid	NdFeO₃/glycine/ carbon nanotubes	0.5–2.5 mmol∙L⁻¹	-	-	106
Ascorbic acid	SrPdO₃	-	-	-	69
Acetaminophen	GdTiO₃/graphene	50 nmol∙L⁻¹–1.5 μmol∙L⁻¹	58.85 nmol∙L⁻¹	2.177 ×10⁻⁵ A·L·nmol⁻¹	105
	LaBO₃ (B = Fe, Co, Ni)	300 nmol∙L⁻¹–27 μmol∙L⁻¹	35 nmol∙L⁻¹	-	117
	LaNi_xCo_1−xO₃	1 μmol∙L⁻¹–0.1 mmol∙L⁻¹	100.0 nmol∙L⁻¹	-	28
Protocatechuic acid	EDAPbCl₄@ZIF-67	22–337 μmol∙L⁻¹	15 μmol∙L⁻¹	-	116

表3

图5

表4

图6

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Detected substance	Key materials	Detection range	Limit of detection	Ref.
Glucose	TiO₂/SrTiO₃/polydopamine/glucose oxidase	0–32 mmol∙L⁻¹	25.68 μmol∙L⁻¹	21
Cysteine	Au/Bi₄NbO₈Cl	0.1–5 mmol∙L⁻¹	10⁻⁵ mol∙L⁻¹	83
Dihydronicotinamide Adenine Dinucleotide	ZnO-inverse opal photonic crystals/CsPbBr₃	0.1–250 μmol∙L⁻¹	0.0120 μmol∙L⁻¹	84
Cholesterol	Molecularly imprinted polymer@polyvinylidene fluoride-MAPbI₃@carbon nanodots	1.0 × 10⁻¹³–5.0 × 10⁻⁸ mol∙L⁻¹	2.1 × 10⁻¹⁴ mol∙L⁻¹	25
miR-155	MAPbI₃/ZnO	1 × 10⁻² fmol∙L⁻¹–2 × 10⁴ pmol∙L⁻¹	5 × 10⁻³ fmol∙L⁻¹	87
Human hepatitis B surface antigen	CsPbBr₃-MoS₂	Order of magnitude of dilution factor 10⁻⁴–1	Dilution factor 4.6 × 10⁻³	85
Human immunodeficiency virus antibody	CsPbBr₃-MoS₂	Order of magnitude of dilution factor 10⁻⁴–1	Dilution factor 2.1 × 10⁻³	85
Alpha fetoprotein	CsPbBr₃-MoS₂	0.1–500 ng∙mL⁻¹	2.7 ng∙mL⁻¹	85
Alpha fetoprotein	TiO₂-inverse opal photonic crystals/CsPbCl₃	0.08–980 ng∙mL⁻¹	30 pg∙mL⁻¹	23
5-hydroxymethylcytosine	Bi₄NbO₈Cl@Bi₂S₃	0.3–300 nmol∙L⁻¹	0.0779 nmol∙L⁻¹	88
Salicylic Acid	Molecularly imprinted polymer/MAPbI₃	7.0 × 10⁻¹³–1.0 × 10⁻⁸ mol∙L⁻¹	1.95 × 10⁻¹³ mol∙L⁻¹	86
Ampicillin	BiFeO₃/graphite-like C₃N₄	1 × 10⁻¹²–1 × 10^–6 mol∙L⁻¹	3.3 × 10⁻¹³ mol∙L⁻¹	89

Detected substance	Key materials	Detection range	Limit of detection	Ref.
Urea	CsPbBr₃@poly (styrene/acrylamide)	1.67 μmol∙L⁻¹–16.67 mmol∙L⁻¹	1.67 μmol∙L⁻¹	99
Humidity	CsPbBr₃	33%–98%	12%	101
Fe³⁺	CsPbBr₃@poly(styrene/acrylamide)	5–150 μmol∙L⁻¹	2.2 μmol∙L⁻¹	30
Fe³⁺	SiO₂@CsPbX₃@SiO₂ (X = Cl⁻, Br⁻, I⁻)	10–70 μmol∙L⁻¹	3 μmol∙L⁻¹	102
Cl⁻	CsPbBr₃	10–130 mmol∙L⁻¹	3 mmol∙L⁻¹	31
Cl⁻	CsPbBr₃/cellulose	-	4.11 mmol∙L⁻¹	26
I^–	CsPbBr₃/cellulose	100 μmol∙L⁻¹–1 mol∙L⁻¹	2.56 mmol∙L⁻¹	26
Omethoate	Molecularly imprinted polymer@CsPbBr₃	50–400 ng∙mL⁻¹	18.8 ng∙mL⁻¹	103
Melittin	CsPbBr₃@Phospholipid	50 nmol∙L⁻¹–150 μmol∙L⁻¹	50 nmol∙L⁻¹	75
Fluoride	MAPbBr₃@n-Octylamine & 6-amino-1-hexanol	10–50 μmol∙L⁻¹	3.2 μmol∙L⁻¹	78
Water content in herbal medicines	CsPbBr₃	1%–17%	Seutellaria baicalensis 0.75%, Astragalus flavone 0.67%	101
Gallic acid	LaFeO₃	0.6–36 μmol∙L⁻¹	0.4 μmol∙L⁻¹	104
Tetracycline	3-aminopropyltriethoxysilane @CsPbBr₃	0.5–15.0 μmol∙L⁻¹	76 nmol∙L⁻¹	24
Tetracycline	CsPbBr₃@BN	0–0.44 mg∙L⁻¹	6.5 ng∙mL⁻¹	100

Substance	Key materials	Operation mechanism	Detection range	Limit of detection	Ref.
Humidity	CsPbBr₃	Physicochemically loading	23%–67%	-	120
Humidity	Cs₂BiAgBr₆	Physicochemically loading	5%–75%	-	119
Volatile biomarkers exhaled by colorectal cancer	SmFeO₃	Physicochemically loading	-	-	126
Carcinoembryonic antigen	LaMnO₃	Physicochemically loading	10⁻⁴–10² ng∙mL⁻¹	3.6 × 10⁻⁴ ng∙mL⁻¹	125
Prostate specific antigen			10⁻⁴–10² ng∙mL⁻¹	2.8 × 10⁻⁴ ng∙mL⁻¹	125
Alpha fetoprotein			10⁻⁴–10² ng∙mL⁻¹	3.4 × 10 ⁻⁴ ng∙mL⁻¹	125
Volatile sulfur compounds	LnFeO₃ (Ln = La, Pr, Nd, Sm)	Physicochemically loading	10–10² ppm	-	29
Glucose	Ag/TiO₂/MAPbX₃/graphene (X = I, Br)	Surface plasmon resonance	10–60 g∙L⁻¹	-	121

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高效医学传感钙钛矿材料研究进展

Recent Advances in High-Efficiency Perovskite for Medical Sensors

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