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Dinuclear Copper Complex for High‐Rate Hydrogen Evolution Under Neutral Aqueous Conditions

机译:中性水条件下高速率析氢的双核铜络合物

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Abstract The development of an efficient and stable electrocatalyst for the hydrogen evolution reaction (HER), based on earth‐abundant components, represents a crucial step toward cost‐effective and environmentally friendly hydrogen production. This study presents the utilization of a dinuclear copper catalyst, denoted as Cu‐Gly‐SB (Complex 1), for HER under both aqueous and non‐aqueous conditions. In non‐aqueous settings, the catalyst achieves excellent HER performance, requiring only a 270 mV overpotential when acetic acid is used as the proton donor. Notably, in fully aqueous conditions, complex 1 attains a remarkable current density of 18.8 mA ⋅ cm−2 at −0.7 V vs. RHE in cyclic voltammetry. The kobs value of ≈2.7×104 s−1 in aqueous solution at pH 7.0 further underlines the superior catalytic performance of 1, outperforming most non‐noble‐metal molecular catalysts functioning in fully aqueous solutions. The robust stability of 1 is demonstrated through controlled potential electrolysis (CPE) over a span of 48 hours, achieving an impressive catalytic current of 11.0 mA ⋅ cm−2 at −0.39 V. Moreover, the catalytic current gradually increases with higher reduction potentials, reaching a substantial 100 mA ⋅ cm−2 at an overpotential of 590 mV during CPE >48 hours. Thorough characterizations further confirm the molecular nature of the catalyst.
机译:摘要 基于地球丰富的组分,开发高效稳定的析氢反应(HER)电催化剂,是迈向经济高效、环境友好的制氢的关键一步。本研究介绍了在水性和非水性条件下利用双核铜催化剂(表示为 [Cu-Gly-SB](配合物 1))处理 HER。在非水环境中,该催化剂可实现出色的 HER 性能,当使用乙酸作为质子供体时,只需要 270 mV 的过电位。值得注意的是,在全水性条件下,配合物1在-0.7 V时达到18.8 mA ⋅ cm−2的显着电流密度,而在循环伏安法中与RHE相比。在pH 7.0的水溶液中,kobs值为≈2.7×104 s−1,进一步强调了1的卓越催化性能,优于在全水溶液中起作用的大多数非贵金属分子催化剂。通过48小时的受控电位电解(CPE)证明了1的稳健稳定性,在−0.39 V时实现了令人印象深刻的11.0 mA ⋅ cm−2催化电流。此外,催化电流随着还原电位的增加而逐渐增加,在CPE>48小时内,在590 mV的过电位下达到100 mA ⋅ cm−2。全面的表征进一步证实了催化剂的分子性质。

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