Three-dimensional ordered porous N-doped carbon-supported accessible Ni-N<subscript>x</subscript> active sites for efficient CO<subscript>2</subscript> electroreduction.
In: Rare Metals, Jg. 42 (2023-06-01), Heft 6, S. 1800-1807
Online
academicJournal
Zugriff:
Electrocatalytic reduction of carbon dioxide (CO 2 RR) into high value-added chemicals and fuels has been regarded as a promising approach to achieve carbon neutrality. Though nickel-nitrogen-carbon (Ni-N-C) electrocatalysts have shown superior CO 2 RR performance, the synthesis of highly effective Ni-N-C catalyst is still challenging. Herein, a three-dimensional (3D) ordered porous nitrogen-doped carbon-supported Ni-N x catalyst has been synthesized by direct pyrolysis of a mixture of SiO 2 , polyvinyl pyrrolidone, nickel-phenanthroline complex, followed by the removal of the SiO 2 templates. Benefiting from the porous structure and accessible active sites, the optimized catalyst exhibits a high CO Faradaic efficiency above 85% between –0.6 and –0.9 V versus reversible hydrogen electrode (vs. RHE), and a large CO current density (j CO ) of –16.2 mA·cm −2 at –0.8 V (vs. RHE). Density functional theory (DFT) calculations demonstrate that the Ni-N-C catalyst with Ni-N x species can enhance CO 2 RR reaction dynamic process and suppress hydrogen evolution reaction, thus improving the conversion efficiency toward CO 2 RR. [ABSTRACT FROM AUTHOR]
摘要: 电催化还原二氧化碳(CO 2 RR)为高附加值的化学品和燃料,是实现碳中和的一个有前景的途径。尽管镍-氮-碳 (Ni-N-C)电催化剂已显示出不错的二氧化碳还原性能,但高效的Ni-N-C 催化剂的合成仍然是一个挑战。在此,通过直接热解二氧化硅、聚乙烯吡咯烷酮、镍-菲罗啉复合物的混合物,然后去除二氧化硅模板,合成了一种Ni-N x 位点锚定的三维(3D)有序多孔的氮掺杂碳支撑的电催化剂。受益于多孔结构和可利用的活性位点,优化后的 催化剂在‒0.6 至‒0.9 V(vs. RHE)之间表现出85%以上的高CO 法拉达效率,并且在‒0.8V 下, CO 电流密度 (jCO),达到‒16.2 mA·cm -2 。密度泛函理论(DFT)计算表明,含有Ni-Nx 位点锚定的Ni-N-C 催化剂可以促进 CO 2 RR 过程,同时抑制析氢反应,从而提高CO 2 RR 催化性能。 [ABSTRACT FROM AUTHOR]
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Titel: |
Three-dimensional ordered porous N-doped carbon-supported accessible Ni-N<subscript>x</subscript> active sites for efficient CO<subscript>2</subscript> electroreduction.
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Autor/in / Beteiligte Person: | Zheng, Si-Jia ; Cheng, Hua ; Yu, Jin ; Bie, Qin ; Chen, Jing-Dong ; Wang, Feng ; Wu, Rui ; Blackwood, Daniel John ; Chen, Jun-Song |
Link: | |
Zeitschrift: | Rare Metals, Jg. 42 (2023-06-01), Heft 6, S. 1800-1807 |
Veröffentlichung: | 2023 |
Medientyp: | academicJournal |
ISSN: | 1001-0521 (print) |
DOI: | 10.1007/s12598-022-02247-z |
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