Modification of the Coordination Environment of Active Sites on MoC for High-Efficiency CH4 Production

doi:10.1002/aenm.202100044

機構典藏 > College of Sciences > Graduate Institute & Department of Physics > Journal Article > Item 987654321/123336

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Title:	Modification of the Coordination Environment of Active Sites on MoC for High-Efficiency CH4 Production
Authors:	Han, Lili;Liu, Xijun;He, Jia;Liang, Zhixiu;Wang, Hsiao-Tsu;Bak, Seong-Min;Zhang, Jingmin;Hunt, Adrian;Waluyo, Iradwikanari;Pong, W. F.;Luo, Jun;Ding, Yi;Adzic, Radoslav R.;Xin, Huolin L.
Keywords:	active sites;CH 4;coordination-environment modification;electrocatalytic CO 2 reduction;OH overadsorption
Date:	2021-04-15
Issue Date:	2023-04-28 17:46:13 (UTC+8)
Publisher:	Wiley-VCH Verlag GmbH & Co. KGaA
Abstract:	Modulating the coordination environment of active sites on catalyst surfaces is crucial to developing effective catalysts and controlling catalysis. However, this may be a highly challenging procedure. Guided by the first-principles calculations, the modification of the coordination environment of active sites on MoC nanoparticle surfaces is experimentally accomplished by anchoring pyridinic N atom rings of holey graphene on Mo atoms. The rings produce electrostatic forces that enable the tuning of the Mo sites′ affinity to reaction intermediates, which passivates Mo hollow sites, activates Mo top sites, and reduces the overadsorption of OH on the Mo active sites, as predicted by calculations. The atomic-level modification is well confirmed by atomic-resolution imaging, high-resolution electron tomography, synchrotron soft X-ray spectroscopy, and operando electrochemical infrared spectroscopy. Consequently, the Faradaic efficiency for CO2 reduction to CH4 is enhanced from 16% to 89%, a record high efficiency so far, in aqueous electrolytes. It also exhibits a negligible activity loss over 50 h.
Relation:	Advanced Energy Materials 11(24), 2100044
DOI:	10.1002/aenm.202100044
Appears in Collections:	[Graduate Institute & Department of Physics] Journal Article

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