Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology , Dalian 116024, China.
ACS Appl Mater Interfaces. 2017 Feb 15;9(6):5302-5311. doi: 10.1021/acsami.6b15402. Epub 2017 Feb 2.
Electrochemical reduction of CO to chemical feedstocks is an attractive solution that prevents CO accumulation in the atmosphere, but it remains a great challenge to develop the cost-effective catalysts. Herein, we synthesized oxide-derived Cu/carbon (OD Cu/C) catalysts by a facile carbonization of Cu-based MOF (HKUST-1). The resulting materials exhibited highly selective CO reduction to alcohol compounds with total faradic efficiencies of 45.2-71.2% at -0.1 to -0.7 V versus reversible hydrogen electrode (RHE). High-yield methanol and ethanol has been achieved on OD Cu/C-1000 with the production rates of 5.1-12.4 and 3.7-13.4 mg L h, respectively. Notably, the onset potential for CHOH formation is near -0.1 V (versus RHE), corresponding to ∼190 mV of overpotential, which is among the lowest overpotentials reported to date for the reduction of CO to CHOH. The improvements in activity and selectivity of the oxide-derived Cu/carbon might be attributed to the synergistic effect between the highly dispersed copper and the matrix of porous carbon. These findings provide a new insight into design of practical catalysts for decreasing atmospheric CO levels and synthesizing liquid fuels.
电化学还原 CO 为化学原料是一种有吸引力的解决方案，可以防止 CO 在大气中的积累，但开发具有成本效益的催化剂仍然是一个巨大的挑战。在此，我们通过简便的碳化 Cu 基 MOF（HKUST-1）合成了衍生氧化物的 Cu/碳（OD Cu/C）催化剂。所得材料在相对于可逆氢电极（RHE）的-0.1 至-0.7 V 下，对醇类化合物具有高度选择性的 CO 还原，总法拉第效率为 45.2-71.2%。在 OD Cu/C-1000 上实现了高产量的甲醇和乙醇，产率分别为 5.1-12.4 和 3.7-13.4 mg L h。值得注意的是，CHOH 形成的起始电位接近-0.1 V（相对于 RHE），对应于约 190 mV 的过电势，这是迄今为止报道的将 CO 还原为 CHOH 的最低过电势之一。衍生氧化物的 Cu/碳的活性和选择性的提高可能归因于高度分散的铜和多孔碳基质之间的协同效应。这些发现为设计用于降低大气 CO 水平和合成液体燃料的实用催化剂提供了新的见解。
