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超薄铋纳米片作为高效 CO 还原电催化剂。

Ultrathin Bismuth Nanosheets as a Highly Efficient CO Reduction Electrocatalyst.

机构信息

Division of Energy Storage, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, P.R. China.

University of Chinese Academy of Sciences, Beijing, 100039, P.R. China.

出版信息

ChemSusChem. 2018 Mar 9;11(5):848-853. doi: 10.1002/cssc.201702229. Epub 2018 Jan 25.

Abstract

Electrochemical reduction of CO to value-added products is an important and challenging reaction for sustainable energy study. Herein, bismuth nanosheets with thickness of around 10 nm were prepared through the electrochemical reduction of Bi . Ultrathin Bi nanosheets with numerous low-coordination sites can efficiently reduce CO to formate in aqueous solution. Within the potential range of -0.9 to -1.2 V vs. reversible hydrogen electrode (RHE), the faradaic efficiency of formate is over 90 %, outperforming many Bi catalysts. At -0.7 V, the Bi nanosheets exhibit much higher current for formate generation than that of bulk Bi, attributed to a high surface area and also modified intrinsic electronic properties brought about by the ultrathin structure. DFT calculations demonstrate that Bi nanosheets have much higher density of states at the Fermi level compared to bulk Bi, favoring improved CO reduction on Bi nanosheets. At -1.0 V, Bi nanosheets exhibit high selectivity for formate and excellent stability during 5 h of electrolysis.

摘要

电化学还原 CO 生成高附加值产物是可持续能源研究中一个重要且具有挑战性的反应。在此,通过电化学还原 Bi 制备了厚度约为 10nm 的铋纳米片。具有大量低配位点的超薄 Bi 纳米片可以有效地将 CO 还原为甲酸盐。在相对于可逆氢电极(RHE)的-0.9 至-1.2 V 的电位范围内,甲酸盐的法拉第效率超过 90%,优于许多 Bi 催化剂。在-0.7 V 时,Bi 纳米片生成甲酸盐的电流比体相 Bi 高得多,这归因于高表面积以及超薄结构带来的固有电子性质的改变。密度泛函理论(DFT)计算表明,与体相 Bi 相比,Bi 纳米片在费米能级处具有更高的态密度,有利于改善 CO 在 Bi 纳米片上的还原。在-1.0 V 时,Bi 纳米片对甲酸盐表现出高选择性和优异的稳定性,在 5 小时的电解过程中没有明显衰减。

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