Qie Liu, Liyuan Gong, Jingjing Wang, Luyao Ma, Yandong Wu, Yu-Cheng Huang, Ta Thi Thuy Nga, Yabin Xu, Zuyao Jiang, Shiqian Du, Hongjing Zhong, Yanjing Wang, Miaoyu Li, Chung-Li Dong, Guobin Wen, Li Tao, Shuangyin Wang
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引用次数: 0
Abstract
The water-gas shift reaction (WGSR) is crucial to the hydrogen economy, which is hampered by the harsh conditions and complicated purification process. In this work, the spatially separated efficient CO conversion and high-purity H2 production are realized by electrochemistry-accelerated water-gas shift reaction (WGSR) with IrN4-RhN4 dual sites single atom catalysts (IrRh-NC) in high-temperature polymer-electrolyte-membrane electrolyzer. In this reaction, the Ir single atoms in the catalysts can rapidly dissociate H2O at an extremely low potential to supply abundant *OH, which ensures the *OH groups bind to the spontaneously adsorbed *CO on neighboring Rh sites to further accelerate CO conversion. What's more, the elevated temperatures (120-300 °C) maintain water in the gaseous state during the reaction, thus greatly facilitating mass transfer of the reactants CO and H2O within the reactor. Employing IrRh-NC as the anodic catalyst, the electrolyzer achieves superior CO catalytic performance (424 mA cm-2 at 0.4 V) and high purity (99.9%) H2 production (3.2 ml min-1), surpassing the performance of particle catalysts. This work illuminates the tantalizing possibility for sustainable hydrogen economic development.
水气转换反应是氢经济的重要组成部分,但其条件苛刻、净化过程复杂,阻碍了氢经济的发展。在高温聚合物-电解质-膜电解槽中,采用IrN4-RhN4双位点单原子催化剂(IrRh-NC),通过电化学加速水气转换反应(WGSR)实现了空间分离的CO高效转化和高纯度H2的生产。在该反应中,催化剂中的Ir单原子可以以极低的电位快速解离H2O,提供丰富的*OH,这保证了*OH基团与邻近Rh位点上自发吸附的*CO结合,进一步加速CO转化。此外,高温(120-300℃)使水在反应过程中保持气态,从而极大地促进了反应物CO和H2O在反应器内的传质。采用IrRh-NC作为阳极催化剂,电解槽具有优异的CO催化性能(0.4 V下424 mA cm-2)和高纯度(99.9%)H2产率(3.2 ml min-1),超过颗粒催化剂的性能。这项工作阐明了可持续氢经济发展的诱人可能性。