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源自ZIF-67的具有增强析氢反应和氧还原反应活性的多孔氮掺杂碳负载的PtCo/Co复合催化剂。

PtCo/Co Composite Catalysts on Porous N-Doped Carbon Support Derived from ZIF-67 with Enhanced HER and ORR Activities.

作者信息

Liu Jiewen, Zhang Jian, Xu Mingjie, Tian Chuanjin, Dong Yanhao, Wang Chang-An

机构信息

School of Materials Science and Engineering, Jingdezhen Ceramic University, Jingdezhen333001, PR China.

State Key Lab of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing100084, PR China.

出版信息

Inorg Chem. 2022 Dec 5;61(48):19309-19318. doi: 10.1021/acs.inorgchem.2c03114. Epub 2022 Nov 16.

Abstract

The primary challenge for efficient H evolution and hydrogen energy conversion is to develop highly active and stable catalysts with simple and reliable preparation processes. In this regard, we have designed and synthesized a porous carbon-supported low-Pt alloy catalyst (PtCo/Co@C composite) using ZIF-67 as a template. It showed uniformly dispersed PtCo/Co on the porous carbon layer due to the confinement effect of the porous carbon layer. PtCo/Co@C demonstrated excellent activity for the hydrogen evolution reaction in the full pH range, with an overpotential of 187 mV in 0.5 M HSO to attain 100 mA/cm as well as long-term stability. It also displayed superior mass activity for the oxygen reduction reaction (ORR) at 0.85 V (vs RHE) compared to the commercial Pt/C. Furthermore, the PtCo/Co@C catalyst exclusively enabled a four-electron reaction process under ORR conditions without the competitive pathway to HO. The current work provides guidance for the design and facile synthesis of Pt-based catalysts with enhanced performance.

摘要

高效析氢反应(H evolution)和氢能转换的主要挑战在于开发具有简单可靠制备工艺的高活性和稳定催化剂。在这方面,我们以ZIF-67为模板设计并合成了一种多孔碳负载的低铂合金催化剂(PtCo/Co@C复合材料)。由于多孔碳层的限域效应,PtCo/Co均匀分散在多孔碳层上。PtCo/Co@C在全pH范围内对析氢反应表现出优异的活性,在0.5 M H₂SO₄中过电位为187 mV时可达到100 mA/cm²,并且具有长期稳定性。与商业Pt/C相比,它在0.85 V(相对于可逆氢电极,vs RHE)下对氧还原反应(ORR)也表现出优异的质量活性。此外,PtCo/Co@C催化剂在ORR条件下仅能实现四电子反应过程,而不存在生成H₂O₂的竞争途径。当前的工作为设计和简便合成具有增强性能的铂基催化剂提供了指导。

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