Unravelling the potential of disposable and modifiable pencils as catalyst supports for hydrogen evolution reaction
Unravelling the potential of disposable and modifiable pencils as catalyst supports for hydrogen evolution reaction
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揭示一次性和可修改铅笔作为析氢反应催化剂载体的潜力
DOI：
10.1039/d2nj03359c
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发表时间：
2022
影响因子：
3.3
通讯作者：
Gupta, Gautam
中科院分区：
文献类型：
--
作者：
Paudel, Mohan;Daniels, Braydan;Arts, Amanda M.;Gupta, Alexander;Kalbfleisch, Theodore;Hofsommer, Dillon T.;Grapperhaus, Craig A.;Buchanan, Robert M.;Gupta, Gautam
日益增长的化石燃料需求和对全球气候变化的日益关注激发了人们对开发电催化剂的兴趣，这些电催化剂通过析氢反应(HER)电解水来生产氢气作为替代的零排放燃料。贵重或非贵重催化剂通常负载在高比表面积的碳材料上，这些载体在HER的热力学和动力学中都起着至关重要的作用。本文评价了分子析氢催化剂二乙酰-双(4-甲基)-3-氨基硫脲Ni(II)(Ni-ATSM)在玻碳、碳糊和铅笔石墨三种不同表面上的电催化活性。在−10 mA cm−2的电流密度下，每个修饰电极的过电位都是基准。碳糊电极的过电位最高(495 MV)。抛光铅笔和玻碳修饰电极的性能相似(GCE的η=395mV，铅笔的η=400mV)。在沉积Ni-ATSM之前，在丙酮中腐蚀一夜的铅笔电极产生最低的过电位(η=354 mV)。电化学阻抗谱证实，刻蚀使石墨界面的电活性表面积增加，电荷转移电阻从275Ω降至50Ω。我们的研究表明，铅笔石墨可以作为评价多相HER催化剂的通用、一次性、经济有效和可重复使用的电极表面。此外，铅笔可以很容易地用台锯切割，以生成新的表面，从而易于对表面进行表征，如电化学、成像和光谱分析。
Increasing fossil fuel demands and growing concerns of global climate change have stimulated interest in the development of electrocatalysts to produce H2 as an alternative zero-emission fuel from the electrolysis of water via hydrogen evolution reaction (HER). Precious or non-precious catalysts are typically loaded on high surface area carbon materials, and these supports play a critical role in both thermodynamics and kinetics of the HER. In this paper, we evaluate the electrocatalytic activity of a molecular hydrogen evolving catalyst, diacetyl-bis(4-methyl)-3-thiosemicarbazone Ni(II) (Ni-ATSM), on three different carbon surfaces: glassy carbon, carbon paste and pencil graphite. The overpotential for each modified electrode was benchmarked at a current density of −10 mA cm−2. Carbon paste electrodes showed highest overpotentials (495 mV) compared to the other electrode surfaces. Polished pencil and glassy carbon modified electrodes performed similarly (η = 395 mV for GCE and η = 400 mV for pencil). Pencil electrodes etched in acetone overnight prior to Ni-ATSM deposition produced lowest overpotentials (η = 354 mV). Etching results in an increase in electroactive surface area and substantial decrease in the charge transfer resistance of the graphitic interface from 275 Ω to 50 Ω, verified using electrochemical impedance spectroscopy (EIS). Our studies demonstrate pencil graphite may serve as versatile, disposable, cost effective, and reproducible electrode surface for the evaluation of heterogeneous HER catalysts. Moreover, pencils can be easily cut with table saw to generate new surface for easy characterization of the surface such as electrochemistry, imaging and spectroscopy.