非酶电化学传感器检测茶碱的最新进展

doi:10.61558/2993-074X.3527

电化学（中英文） ›› 2025, Vol. 31 ›› Issue (3): 2411291. doi: 10.61558/2993-074X.3527

非酶电化学传感器检测茶碱的最新进展

Gustria Ernis^a^,^b, Yulia M T A Putri^a, Muhammad Iqbal Syauqi^c, Prastika Krisma Jiwanti^d, Yeni Wahyuni Hartati^e, Takeshi Kondo^f, Qonita Kurnia Anjani^g, Jarnuzi Gunlazuardi^a^,^*()

^a印度尼西亚大学数学与自然科学学院化学系，雅加达 16425，印度尼西亚
^b明古鲁大学数学与自然科学学院科学实验室系，明古鲁 38112，印度尼西亚
^c国家研究和创新署化学研究中心，坦格朗 15314，印度尼西亚
^d艾尔朗加大学先进技术与多学科纳米技术工程学院，泗水 60115，印度尼西亚
^e巴查查兰大学数学与自然科学学院化学系，贾蒂南戈尔 45363，印度尼西亚
^f东京理科大学纯粹与应用化学系，野田，278-8510，日本
^g贝尔法斯特女王大学药学院，医学生物学中心，97利斯本路，贝尔法斯特 BT9 7BL，英国

收稿日期:2024-11-28 修回日期:2025-02-02 接受日期:2025-02-17 发布日期:2025-02-18 出版日期:2025-03-28

Recent Advances in Non-Enzymatic Electrochemical Sensors for Theophylline Detection

Ernis Gustria^a^,^b, Putri Yulia M T A^a, Syauqi Muhammad Iqbal^c, Jiwanti Prastika Krisma^d, Hartati Yeni Wahyuni^e, Kondo Takeshi^f, Anjani Qonita Kurnia^g, Gunlazuardi Jarnuzi^a^,^*()

^aDepartment of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Indonesia, Kampus UI Depok, Jakarta 16-42Indonesia
^bDepartment of Science Laboratory, Faculty of Mathematics and Natural Sciences, Universitas Bengkulu, Jl. WR. Supratman, Kandang Limun, Bengkulu City, 38112, Indonesia
^cResearch Center for Chemistry, National Research and Innovation Agency, B. J. Habibie Science and Technology Area, South Tangerang, 15314, Indonesia
^dNanotechnology Engineering, Faculty of Advanced Technology and Multidiscipline, Universitas Airlangga, Surabaya 60115, Indonesia
^eDepartment of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Padjajaran, Jatinangor 45363, Indonesia
^fDepartment of Pure and Applied Chemistry, Tokyo University of Science, 2641 Yamazaki, Noda 278-8510, Chiba, Japan
^gSchool of Pharmacy, Medical Biology Centre, Queen’s University Belfast, 97 Lisburn Road, Belfast BT9 7BL, UK

Received:2024-11-28 Revised:2025-02-02 Accepted:2025-02-17 Online:2025-02-18 Published:2025-03-28
Contact: *E-mail: jarnuzi@ui.ac.id

摘要/Abstract

摘要： 低浓度目标分析物的检测在制药、医疗保健和环境保护等各个领域具有重要意义。茶碱是一种天然生物碱，作为支气管扩张剂，可用于治疗哮喘、支气管炎和肺气肿等呼吸系统疾病，但治疗窗口较窄，成年人的安全血药浓度范围仅为55.5~111.0 µmol·L^-1，太低或太高都会导致严重的副作用。因此，准确监测茶碱水平至关重要。非酶电化学传感器可提供一种快速、便携和高灵敏度的实用解决方案。本文旨在对用于茶碱检测的非酶电化学传感器的最新进展进行全面综述，重点介绍其基本原理、电氧化机制、催化效应以及改性材料对电极性能的作用。本文指出了各种改性材料的重要贡献，包括碳纳米管、石墨烯、金属氧化物和多元纳米复合材料等纳米材料，深入讨论了茶碱的电氧化机理，强调了羟基和羰基反应途径受pH和电极材料的强烈影响，以及应用于指导针对特定应用选择适当的电极材料，从而提高非酶电化学传感器性能的优质改性材料的策略。结果表明，基于二氧化钛、碳纳米管和金纳米颗粒制备的多元纳米复合材料可得到3 × 10⁻⁵ µmol·L^-1的最低检测限，表明在开发高性能电化学传感器方面的巨大潜力。本文的主要结论是电极材料设计中多学科方法对于支持茶碱检测的灵敏度和选择性的重要性。尽管该领域研究已取得显著进展，但在理解茶碱更详细的氧化机制方面仍存在研究空白，特别是在pH变化和复杂环境下的茶碱电氧化机理研究面临挑战。因此，迫切需要进一步研究电极修饰和茶碱氧化机理分析，以提高传感器的准确性和稳定性，同时扩大其在药物监测和医疗诊断中的应用。通过整合各种新材料和技术方法，这篇综述有望为开发高效且经济实用的非酶电化学传感器提供重要参考。

关键词: 茶碱测定, 非酶传感器, 电化学传感器, 电极改性剂, 反应机制

Abstract:

Detection of target analytes at low concentrations is significant in various fields, including pharmaceuticals, healthcare, and environmental protection. Theophylline (TP), a natural alkaloid used as a bronchodilator to treat respiratory disorders such as asthma, bronchitis, and emphysema, has a narrow therapeutic window with a safe plasma concentration ranging from 55.5-111.0 µmol·L^-1 in adults. Accurate monitoring of TP levels is essential because too low or too high can cause serious side effects. In this regard, non-enzymatic electrochemical sensors offer a practical solution with rapidity, portability, and high sensitivity. This article aims to provide a comprehensive review of the recent developments of non-enzymatic electrochemical sensors for TP detection, highlighting the basic principles, electro-oxidation mechanisms, catalytic effects, and the role of modifying materials on electrode performance. Carbon-based electrodes such as glassy carbon electrodes (GCEs), carbon paste electrodes (CPEs), and carbon screen-printed electrodes (SPCEs) have become the primary choices for non-enzymatic sensors due to their chemical stability, low cost, and flexibility in modification. This article identifies the significant contribution of various modifying materials, including nanomaterials such as carbon nanotubes (CNTs), graphene, metal oxides, and multi-element nanocomposites. These modifications enhance sensors' electron transfer, sensitivity, and selectivity in detecting TP at low concentrations in complex media such as blood plasma and pharmaceutical samples. The electro-oxidation mechanism of TP is also discussed in depth, emphasizing the hydroxyl and carbonyl reaction pathways strongly influenced by pH and electrode materials. These mechanisms guide the selection of the appropriate electrode material for a particular application. The main contribution of this article is to identify superior modifying materials that can improve the performance of non-enzymatic electrochemical sensors. In a recent study, the combination of multi-element nanocomposites based on titanium dioxide(TiO₂), CNTs, and gold nanoparticles(AuNPs) resulted in the lowest detection limit of 3 × 10^-5 µmol·L^-1, reflecting the great potential of these materials for developing high-performance electrochemical sensors. The main conclusion of this article is the importance of a multidisciplinary approach in electrode material design to support the sensitivity and selectivity of TP detection. In addition, there is still a research gap in understanding TP's more detailed oxidation mechanism, especially under pH variations and complex environments. Therefore, further research on electrode modification and analysis of the TP oxidation mechanism are urgently needed to improve the accuracy and stability of the sensor while expanding its applications in pharmaceutical monitoring and medical diagnostics. By integrating various innovative materials and technical approaches, this review is expected to be an essential reference for developing efficient and affordable non-enzymatic electrochemical sensors.

Key words: Theophylline detection, Non-enzymatic sensors, Electrochemical sensors, Modifier electrode, Reaction mechanism

Gustria Ernis, Yulia M T A Putri, Muhammad Iqbal Syauqi, Prastika Krisma Jiwanti, Yeni Wahyuni Hartati, Takeshi Kondo, Qonita Kurnia Anjani, Jarnuzi Gunlazuardi. 非酶电化学传感器检测茶碱的最新进展[J]. 电化学（中英文）, 2025, 31(3): 2411291.

Ernis Gustria, Putri Yulia M T A, Syauqi Muhammad Iqbal, Jiwanti Prastika Krisma, Hartati Yeni Wahyuni, Kondo Takeshi, Anjani Qonita Kurnia, Gunlazuardi Jarnuzi. Recent Advances in Non-Enzymatic Electrochemical Sensors for Theophylline Detection[J]. Journal of Electrochemistry, 2025, 31(3): 2411291.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.61558/2993-074X.3527

https://electrochem.xmu.edu.cn/CN/Y2025/V31/I3/2411291

图/表 10

Electrode Modifier	Method	LOD(µmol·L^-1)	Linearity(µmol·L^-1)	Medium	pH	Mechanism route	Real sample	Ref.
Unmodified (GCE bare)	SWV DPV	0.0130 0.0860	0.1-100 0.1-100	Acetate buffer	4.5	Hydroxyl	drug tablet	[74]
WO₃/MWCNT	CV, DPV	0.0080	0.025-2.6	H₂SO₄	1.3	Carbonyl	pharmaceutical tablet and urine samples	[49]
TCPP(Ni)-Co	DPV	0.0033	0.01-0.1	Na₂HPO₄-C₄H₂O₇	3.5	Carbonyl	tea drinks	[82]
GNP-CHIT-IL hybrid/r-GO	CV, DPV	0.0132	0.025-2.1	PBS	7.4	—	tea, energy drink, green tea, human urine and serum	[83]
PLCY/N-CNT	CV, DPV	0.0330	0.1-70.0	H₂SO₄-Na₂SO₄	1.7	Hydroxyl	green tee, oral TP sustained-release tablets	[79]
Ca₂CuO₃	CV, DPV	0.1050	0.250-2070	PBS	7.0	Hydroxyl, Carbonyl	human urine and serum samples	[76]
LV@CNF	amperometry(i-t)	0.0026	0.01-1070	PBS	7.0	Hydroxyl	chocolate, coffee, black tea	[84]
MoS₂/PANI@g-C₃N₄	DPV	0.0500	6.6-98	PBS	7.0	Hydroxyl	foodstuff, energy drinks, and pharma products.	[80]
TiO₂ NPs	DPV	0.0230	0.023-0.2	PBS	6.0	Hydroxyl	drug tablets, urine	[70]
TiO₂ MPs	Amperometric	0.0133	0.02-209.6	PBS	7.0	Carbonyl	serum, drug tablets	[75]
ns-ZSO	DPV	0.0030	0.02-0.6	PBS	7.0	Carbonyl	blood serum, oranges, tea, coffee, and chocolate	[85]
GCO-gCN	CV, DPV	0.0533	0.0001-0.003	PBS	7.0	Carbonyl	tea, oranges, chocolate, coffee, and human blood serum	[65]
P(L-Asp)/f-MWCNT	SWV	0.0200	0.1-50	PBS	6.0	—	panadol extra pharmaceutical formulation samples, blood serum, and green tea	[86]
Gd₂(MoO₄)₃ nanosheets	DPV	0.0119	0.03 - 1.5	PBS	7.0	Hydroxyl	green tea drink and the urine samples	[71]
AFW/Nf	CV, DPV	2.8000	100-160000	PBS	7.0	—	human serum, black tea, and urine samples	[87]
WS₂ nano-flowers/Ag NPs composites	DPV	0.0030	0.05-150	H₂SO₄	1.0	—	tea samples and pharmaceutical tablets	[88]
CdS/PTA/Nafion	DPV	0.6000	1-200	PBS	8.0	—	urine	[59]
CNOs	DPV	0.3500	8.16-108.25	PBS	7.0	—	human serum	[89]
AuNP-MWCNT	DPV	0.0900	0.5-20	Britton-Robison(BR) buffer	6.0	Carbonyl	pharmaceutical tablets and tea samples	[90]
La₂O₃/MWCNT nanocomposite	DPV	0.0100	0.1-400.0	PBS	7.0	—	human blood, serum, and urine samples	[77]
pPABSA	SWV	7.0200	10-100	PBS	7.0	Carbonyl Hydroxyl	tea and coffee	[91]
DMN-AuNPs	CV, DPV	0.0096	0.05-2	H₂SO₄	7.0	—	tea and biological samples	[92]
RGO- SDS- Nafion composite film	CV, DPV	0.0050	0.01-0.10, 0.1-1.0, and 1.0-40	H₂SO₄	2-6	Carbonyl	pharmaceutical samples	[93]
MWNT\|MnO₂	DPV	0.0100	0.1-20	PBS	6.0	Hydroxyl	pharmaceutical sample and green tea	[93]
PAMT/AuNPs/TiO₂@CuO-B/RGO	DPV	3 × 10^-5	0.00008-1	ABS	4.0	—	real blood serum	[81]
(poly(PRO)-MWCNTs	DPV	0.0400	9.66-100.5	PBS	3.0	—	tea, coffee, yerba mate infusion, energy drink	[46]
NiF/AC	CV	0.2100	0.5-5	BRS	3.0	Hydroxyl	human urine	[94]
Chit/NH₂-IL/MnO_x	CV	0.0500	0.2-120	ABS	5.0	Hydroxyl	—	[69]

Electrode Modifier	Method	LOD (μmol·L^-1)	Linearity (μmol·L^-1)	Medium	pH	Mechanism route	Real Sample	Ref.
MWCNTs	CV, SWV	0.1940	0.8-90	Britton Robinson buffer	3.0	—	plasma samples	[96]
1E3MICl/ Fe₃O₄/SWCNTs	CV, SWV	0.0500	0.1-300.0	PBS	6.0	—	Fish, meat, tea, and soft drinks.	[101]
Nano-CoPc	DPV	0.1400	0.4-100	PBS	7.4	—	Drug tablets, green tea	[102]
CTAB	DPV	0.1850	0.08-200	PBS	3.0	Hydroxyl	Drug tablets, urine	[100]
MWCNT	DPV	0.0197	2-150	Britton-Robinson(BR) buffer	3.0	Hydroxyl	Drug tablets, urine	[51]
EFTAG	SWV	15	20-1000	PBS	7.0	—	Human blood serum, urine	[45]
MWCNT/CuO	Potentiometric	0.0250	0.1 - 10,000	PBS	6.0	—	Chinese black tea, Chinese green tea, Indian black tea, Indian green tea.	[97]
SiO₂@TiO₂@poly(MAA − EGDMA)	DPV	0.0012	0.010-40	PBS	6.5	—	tea, human blood serum, and urine	[44]
CuO-GO	CV, DPV	0.0083	0.1-3.5	PBS	6.0	Hydroxyl	Urine	[98]
CHL-GO	LSV	0.0044	0.03-500	PBS	6.0	Hydroxyl	Drug sample	[99]
MIPs	DPV	0.0024	5-15	Buffer Saline	7.4	—	Human blood sample	[103]

Electrode	Electrode Modifier	Method	LOD(μmol·L^-1)	Linearity(μmol·L^-1)	Medium	pH	Mechanism route	Real Sample	Ref.
BDD	—	LSV	—	1-400	buffer solution containing NaClO₄	1.8	—	coffee and cola	[113]
BDD	—	DPV SWV	0.9100 1.4500	2-380	H₂SO₄	1.5	—	pharmaceuticals, human urine	[52]
BDD	NiNPs	SWV, CV	2.7900	30-100	PBS	3.0	hydroxyl	artificial urine	[68]
CFE	—	CV, FSV	0.5000	0.50-30	PBS	7.4	—	coffee	[119]
PGE	CTAB	CV, DPV	0.0026	0.1-1.3	PBS	2.0	Hydroxyl	tablet and urine samples	[115]
PGE	NiO/MWCNT/NNaM	CV, DPV	0.3610	5-200	Britton-Robinson buffer	2.0	—	human urine, black tea, Earl Grey, and bitter chocolate	[116]
CBE	PLA (polylactic acid)	SWV	1.2000	5-150	PBS	7.0	—	TP tablets and artificial urine	[120]

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非酶电化学传感器检测茶碱的最新进展

Recent Advances in Non-Enzymatic Electrochemical Sensors for Theophylline Detection

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Metrics

Electrode Modifier	Method	LOD (μM)	Linearity(μM)	Medium	pH	Mechanism route	Real Sample	Ref.
Unmodified (SPCE bare)	CV	10	55-100	PBS	7.4	Carbonyl Hydroxyl	—	[4]
b-NiS/Ppy	SWV	0.0010	0.01-900000	PBS	6.0	—	human urine, serum, and fresh tea leaf extracts	[107]
RuOx -FSWCNT	Amperometric	0.0010	0.005-500	H₂SO₄	—	Carbonyl	drug tablets	[64]
GQD	DPV	0.200	1-700	PBS	7.0	Hydroxyl	oral solution, urine	[48]
BiOBr	DPV Amperometric	0.00072 0.00035	0.001-2.011 0.002-1.48	PBS	7.0	Carbonyl	orange Juice	[106]
DNA aptamer-BDD-Au	DPV	0.052	1-100	PBS	7.4	—	blood serum	[108]

Electrode	Electrode Modifier	Method	LOD (μmol·L^-1)	Linearity (µmol·L^-1)	Medium	pH	Mechanism route	Real Sample	Ref.
Au	AuNPs/Aptamer	SWV	0. 0700	0.1-80	tris-HCl buffer	7.5	—	serum	[121]
Au	AgNPs/Aptamer	LSV	0.0500	0.50-70	PBS	7.4	—	serum	[7]
Au	MIP(Phenol)	Capacitance	1	1-15	borate buffer solution	9.2	—	—	[122]
ITO	MIP(MAA-EGDMA)	CV	—	2000- 4000	aqueous	7.0	—	—	[124]
ITO and Si	MIP(MAA-EGDMA)	CV	—	—	aqueous	7.0	—	aqueous	[123]