Liu Shengwen, Wang Maoyu, Yang Xiaoxuan, Shi Qiurong, Qiao Zhi, Lucero Marcos, Ma Qing, More Karren L, Cullen David A, Feng Zhenxing, Wu Gang
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR, 97331, USA.
Angew Chem Int Ed Engl. 2020 Nov 23;59(48):21698-21705. doi: 10.1002/anie.202009331. Epub 2020 Sep 23.
Atomically dispersed and nitrogen coordinated single metal sites (M-N-C, M=Fe, Co, Ni, Mn) are the popular platinum group-metal (PGM)-free catalysts for many electrochemical reactions. Traditional wet-chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M-N-C catalysts. The deposition of gaseous 2-methylimidazole onto M-doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD-derived Fe-N-C catalyst exclusively contains atomically dispersed FeN sites with increased Fe loading relative to other catalysts from wet-chemistry synthesis. The catalyst exhibited outstanding oxygen-reduction activity in acidic electrolytes, which was further studied in proton-exchange membrane fuel cells with encouraging performance.
原子分散且氮配位的单金属位点(M-N-C,M = Fe、Co、Ni、Mn)是用于许多电化学反应的流行的无铂族金属(PGM)催化剂。传统的湿化学催化剂合成通常需要复杂的程序,且重现性和可扩展性不尽人意。在此,我们报告了一种简便的化学气相沉积(CVD)策略来合成有前景的M-N-C催化剂。将气态2-甲基咪唑沉积到M掺杂的ZnO衬底上,随后进行原位热活化,有效地生成了很好地分散在多孔碳中的单金属位点。特别地,一种最佳的CVD衍生的Fe-N-C催化剂仅包含原子分散的FeN位点,相对于湿化学合成的其他催化剂,其铁负载量有所增加。该催化剂在酸性电解质中表现出出色的氧还原活性,并在质子交换膜燃料电池中进行了进一步研究,性能令人鼓舞。