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用于在气相中使用Nafion-H电解质将CO选择性还原为CO的Co-N-C电催化剂的活性中心

The Active Center of Co-N-C Electrocatalysts for the Selective Reduction of CO to CO Using a Nafion-H Electrolyte in the Gas Phase.

作者信息

Ogihara Hitoshi, Maezuru Tomomi, Ogishima Yuji, Inami Yuta, Saito Mayuko, Iguchi Shoji, Yamanaka Ichiro

机构信息

Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, Ookayama, Meguro-Ku, Tokyo 1528552, Japan.

Department of Applied Chemistry, Saitama University, Shimo-Ookubo, Saitama 3388570, Japan.

出版信息

ACS Omega. 2020 Aug 3;5(31):19453-19463. doi: 10.1021/acsomega.0c01510. eCollection 2020 Aug 11.

DOI:10.1021/acsomega.0c01510
PMID:32803039
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7424585/
Abstract

To contribute a solution for the global warming problem, the selective electrochemical reduction of CO to CO was studied in the gas phase using a [CO(g), Co-N-C cathode | Nafion-H | Pt/C anode, H/water] system without using carbonate solutions. The Co-N-C electrocatalysts were synthesized by partial pyrolysis of precursors in inert gas, which were prepared from various N-bidentate ligands, Co(NO), and Ketjenblack (KB). The most active electrocatalyst was Co-(4,4'-dimethyl-2,2'-bipyridine)/KB pyrolyzed at 673 K, denoted Co-4,4'-dmbpy/KB(673K). A high performance of CO formation (331 μmol h cm, 217 TOF h) at 0.020 A cm with 78% current efficiency was obtained at -0.75 V (SHE) and 273 K under strong acidic conditions of Nafion-H. Characterization studies using extended X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy-energy-dispersive X-ray (TEM-EDX), X-ray diffraction (XRD), and temperature-programmed desorption with mass spectrometry (TPD-MS) indicated the active site as Co coordinated with four N atoms bonding the surface of KB, abbreviated Co-N-C structure. A model of the reduction mechanism of CO on the active site was proposed.

摘要

为了找到全球变暖问题的解决方案，我们研究了在气相中使用[CO(g)，Co-N-C阴极|Nafion-H|Pt/C阳极，H/水]系统将CO选择性电化学还原为CO的过程，该过程不使用碳酸盐溶液。Co-N-C电催化剂是通过前驱体在惰性气体中部分热解合成的，前驱体由各种N-双齿配体、Co(NO)和科琴黑(KB)制备而成。活性最高的电催化剂是在673K下热解的Co-(4,4'-二甲基-2,2'-联吡啶)/KB，记为Co-4,4'-dmbpy/KB(673K)。在Nafion-H的强酸性条件下，于-0.75V(SHE)和273K时，在0.020A cm下获得了331μmol h cm的CO生成高性能，电流效率为78%，TOF为217 h。使用扩展X射线吸收精细结构(EXAFS)、X射线光电子能谱(XPS)、透射电子显微镜-能量色散X射线(TEM-EDX)、X射线衍射(XRD)以及程序升温脱附质谱(TPD-MS)进行的表征研究表明，活性位点是与四个N原子配位的Co，这些N原子键合在KB表面，简称为Co-N-C结构。提出了活性位点上CO还原机理的模型。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/acffd54a6f9d/ao0c01510_0010.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/77a9e3b55a6c/ao0c01510_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/77f206339c0a/ao0c01510_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/6695357f819f/ao0c01510_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/66943746fb85/ao0c01510_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2dbe/7424585/acffd54a6f9d/ao0c01510_0010.jpg

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