DataVXAdvanced Functional MaterialsPaper
journal article·2021-12Open access

Molecular Engineering to Tune the Ligand Environment of Atomically Dispersed Nickel for Efficient Alcohol Electrochemical Oxidation

Zhifu Liang, Daochuan Jiang, Xiang Wang, Mohsen Shakouri, Ting Zhang, Zhongjun Li, Pengyi Tang, Jordi Llorca, Lijia Liu, Yupeng Yuan, Marc Heggen, Rafal E. Dunin‐Borkowski, Joan R. Morante, Andreu Cabot, Jordi Arbiol

Advanced Functional Materials· Volume 31· Issue 51
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Source abstract

Abstract

Abstract Atomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catalysts through the modification of their edge coordination is an effective strategy to maximize their performance. This article focuses on optimizing nickel‐based electrocatalysts toward alcohol electrooxidation in alkaline solution. A new organic framework with atomically dispersed nickel is first developed. The coordination environment of nickel within this framework is modified through the addition of carbonyl (CO) groups. The authors then demonstrate that such nickel‐based organic frameworks, combined with carbon nanotubes, exhibit outstanding catalytic activity and durability toward the oxidation of methanol (CH3OH), ethanol (CH3CH2OH), and benzyl alcohol (C6H5CH2OH); the smaller molecule exhibits higher catalytic performance. These outstanding electrocatalytic activities for alcohol electrooxidation are attributed to the presence of the carbonyl group in the ligand chemical environment, which enhances the adsorption for alcohol, as revealed by density functional theory calculations. The work not only introduces a new atomically dispersed Ni‐based catalyst, but also demonstrates a new strategy for designing and engineering high‐performance catalysts through the tuning of their chemical environment.
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Research context

NanomaterialsCatalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Covalent Organic Framework Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Catalan Institute of Nanoscience and Nanotechnology (ICN2) CSIC and BIST Campus UAB, Bellaterra Barcelona Catalonia 08193 Spain

Functional Nanomaterials Group Catalonia Institute for Energy Research – IREC Sant Adrià de Besòs Barcelona Catalonia 08930 Spain

School of Chemistry and Chemical Engineering Anhui University Heifei Anhui 230601 China

Canadian Light Source Saskatoon S7N 0X4 Canada

School of Physics Hefei University of Technology Hefei 230009 P. R. China

State Key Laboratory of Information Functional Materials, 2020 X‐Lab Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai 200050 China

Ernst Ruska‐Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute Forschungszentrum Jülich GmbH 52425 Jülich Germany

Institute of Energy Technologies Department of Chemical Engineering and Barcelona Research Center in Multiscale Science and Engineering Universitat Politècnica de Catalunya EEBE Barcelona Catalonia 08019 Spain

Department of Chemistry Western University 1151 Richmond Street London ON N6A5B7 Canada

ICREA Pg. Lluís Companys 23 Barcelona Catalonia 08010 Spain

Funding

European Regional Development Fund · China Scholarship Council · Natural Sciences and Engineering Research Council of Canada · Alexander von Humboldt-Stiftung · Generalitat de Catalunya · Ministerio de Economía, Industria y Competitividad, Gobierno de España · Horizon 2020 Framework Programme · Ministerio de Ciencia Tecnología y Telecomunicaciones

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