期刊
CHEMICAL ENGINEERING JOURNAL
卷 446, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136927
关键词
Dopamine; Nanoporous Diamond; Surface engineering; Gold nanoparticles
资金
- National Key Research and Development Program of China [2021YFB3701800, 2016YFB0301400]
- Na-tional Natural Science Foundation of China [52071345, 51874370]
- Province Key Research and Development Program of Guangdong [2020B010185001]
- Province High-tech Industry Science and Technology Innovation Leading Plan of Hunan [2022GK4037, 2022GK4047]
- State Key Laboratory of Pow-der Metallurgy
In this study, a fouling-resistant nanoporous diamond sensing interface called NanoDiaSens was engineered. It allows reliable voltammetric quantification of the target substance dopamine in human serum. NanoDiaSens possesses stable electroactive gold nanoparticles and the capability to eliminate the response of interfering substances, exhibiting excellent electrocatalytic properties.
Electrode fouling is an inevitable phenomenon when encountering biological agents (e.g., dopamine, peptides, proteins), particularly working under continuous oxidation of fouling agents. Diamond is emerging as an ideal fouling-resistant sensing material due to favorable antifouling properties and biocompatibility, but the detection sensitivity and specificity narrow its biomedical applications. In this work, we engineered a Au-NPs/Nafion modified nanoporous diamond sensing interface (termed as NanoDiaSens) in which the target's voltammetric response (i.e., dopamine) is dominant while interference agents (i.e., human serum, ascorbic acid) are eliminated, rendering reliable target quantification in human serum. The resulting nanopores and electrodeposited Au NPs have close size distribution of 43.1 +/- 9.2 nm and 43.9 +/- 12.7 nm respectively. The unique nanoporous diamond sensing surface provides anchored sites to stabilize electroactive gold nanoparticles preserving their long lifespan and high sensitivity, while surface-modified Nafion membrane effectively eliminates the voltammetric response of the interference agents and shifts the target's potential window away from the interferent's ones, achieving specific voltammetric quantification of the target. The NanoDiaSens also holds the highest heterogeneous kinetic constant of 6.7 x 10-3 cm s- 1, indicating the significantly enhanced electrocatalytic properties. Leveraging NanoDiaSens, we realized high accuracy of > 90% recovery rate for dopamine's voltammetric response currents over wide levels (from 3 to 100 mu M) in human serum. NanoDiaSens preserves the reliable voltammetric signals within 2.1% signal attenuation up to one month and maintains 95% of the initial response current after six-month storage in the ambient environment. We expect NanoDiaSens holds the potentials for personalized dopamine monitoring for many months.
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