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A rational study on the geometric and electronic properties of single-atom catalysts for enhanced catalytic performance

DOI: 10.1039/D0NR06006B DOI Help

Authors: Qi Xue (The Hong Kong Polytechnic University Shenzhen Research Institute) , Yi Xie (The Chinese University of Hong Kong) , Simson Wu (University of Oxford) , Tai-sing Wu (National Tsing Hua University) , Yun-liang Soo (National Tsing Hua University) , Sarah Day (Diamond Light Source) , Chiu C. Tang (Diamond Light Source) , Ho W. Man (The Hong Kong Polytechnic University Shenzhen Research Institute) , Sha T. Yuen (The Chinese University of Hong Kong) , Kwok-yin Wong (The Hong Kong Polytechnic University Shenzhen Research Institute) , Yin Wang (The Chinese University of Hong Kong) , Benedict T. W. Lo (The Hong Kong Polytechnic University Shenzhen Research Institute; The Hong Kong Polytechnic University) , Shik C. E. Tsang (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nanoscale , VOL 4

State: Published (Approved)
Published: October 2020
Diamond Proposal Number(s): 23230

Abstract: We investigate the geometric and electronic properties of single-atom catalysts (SACs) within metal–organic frameworks (MOFs) with respect to electrocatalytic CO2 reduction as a model reaction. A series of mid-to-late 3d transition metals have been immobilised within the microporous cavity of UiO-66-NH2. By employing Rietveld refinement of new-generation synchrotron diffraction, we not only identified the crystallographic and atomic parameters of the SACs that are stabilised with a robust M⋯N(MOF) bonding of ca. 2.0 Å, but also elucidated the end-on coordination geometry with CO2. A volcano trend in the FEs of CO has been observed. In particular, the confinement effect within the rigid MOF can greatly facilitate redox hopping between the Cu SACs, rendering high FEs of CH4 and C2H4 at a current density of −100 mA cm−2. Although only demonstrated in selected SACs within UiO-66-NH2, this study sheds light on the rational engineering of molecular interactions(s) with SACs for the sustainable provision of fine chemicals.

Subject Areas: Physics, Chemistry


Instruments: I11-High Resolution Powder Diffraction

Other Facilities: SPring-8; Taiwan Photon Source (TPS)