Li Yang, Wang Xian, Mei Bingbao, Wang Ying, Luo Zhaoyan, Luo Ergui, Yang Xiaolong, Shi Zhaoping, Liang Liang, Jin Zhao, Wu Zhijian, Jiang Zheng, Liu Changpeng, Xing Wei, Ge Junjie
State Key Laboratory of Electroanalytic Chemistry, Jilin Province Key Laboratory of Low Carbon Chemistry Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China; University of Chinese Academy of Sciences, Beijing 100049, China.
Sci Bull (Beijing). 2021 Jul 15;66(13):1305-1311. doi: 10.1016/j.scib.2021.02.006. Epub 2021 Feb 6.
Proton exchange membrane fuel cells (PEMFCs) suffer extreme CO poisoning even at PPM level (<10 ppm), owning to the preferential CO adsorption and the consequential blockage of the catalyst surface. Herein, however, we report that CO itself can become an easily convertible fuel in PEMFC using atomically dispersed Rh catalysts (Rh-N-C). With CO to CO conversion initiates at 0 V, pure CO powered fuel cell attains unprecedented power density at 236 mW cm, with maximum CO turnover frequency (64.65 s, 363 K) far exceeding any chemical or electrochemical catalysts reported. Moreover, this feature enables efficient CO selective removal from H gas stream through the PEMFC technique, with CO concentration reduced by one order of magnitude through running only one single cell, while simultaneously harvesting electricity. We attribute such catalytic behavior to the weak CO adsorption and the co-activation of HO due to the interplay between two adjacent Rh sites.
质子交换膜燃料电池(PEMFCs)即使在百万分之一水平(<10 ppm)下也会遭受严重的一氧化碳中毒,这是由于一氧化碳的优先吸附以及随之而来的催化剂表面堵塞。然而,在此我们报告,在使用原子分散的铑催化剂(Rh-N-C)的质子交换膜燃料电池中,一氧化碳本身可以成为一种易于转化的燃料。一氧化碳到一氧化碳的转化在0 V时开始,纯一氧化碳驱动的燃料电池在236 mW/cm²时达到了前所未有的功率密度,最大一氧化碳周转频率(64.65 s⁻¹,363 K)远远超过了所报道的任何化学或电化学催化剂。此外,这一特性使得通过质子交换膜燃料电池技术能够从氢气气流中高效选择性地去除一氧化碳,仅通过运行单个电池就能使一氧化碳浓度降低一个数量级,同时还能发电。我们将这种催化行为归因于两个相邻铑位点之间的相互作用导致的一氧化碳弱吸附和水的共活化。