Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
Liang, Zhifu (Institut Català de Nanociència i Nanotecnologia)
Jiang, Daochuan (Anhui University. School of Chemistry and Chemical Engineering)
Wang, Xiang (Institut de Recerca en Energia de Catalunya)
Shakouri, Mohsen (Canadian Light Source)
Zhang, Ting (Institut Català de Nanociència i Nanotecnologia)
Li, Zhongjun (Hefei University of Technology. School of Physics.)
Tang, PengYi (Shanghai Institute of Microsystem and Information Technology)
Llorca, Jordi (Universitat Politècnica de Catalunya. Departament d'Enginyeria Química)
Liu, Lijia (Western University. Department of Chemistry)
Yuan, Yupeng (Anhui University. School of Chemistry and Chemical Engineering)
Heggen, Marc (Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons (Jülich, Alemanya))
Dunin-Borkowski, Rafal E. (Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons (Jülich, Alemanya))
Morante, Joan Ramon (Institut de Recerca en Energia de Catalunya)
Cabot, Andreu (Institució Catalana de Recerca i Estudis Avançats)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)

Fecha:	2021
Resumen:	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 (CO) 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 (CHOH), ethanol (CHCHOH), and benzyl alcohol (CHCHOH); 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.
Ayudas:	European Commission 823717 Ministerio de Ciencia e Innovación RTI2018-093996-B-C31 Ministerio de Economía y Competitividad PID2020-116093RB-C43 Ministerio de Economía y Competitividad SEV-2017-0706 Ministerio de Economía y Competitividad ENE2017-85087-C3 Ministerio de Economía y Competitividad ENE2016-77798-C4-3-R Ministerio de Economía y Competitividad SEV-2013-0295-17-1 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1246 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-327 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-128
Nota:	Altres ajuts: ICN2 is funded by the CERCA Programme /Generalitat de Catalunya. Part of the present work has been performed in the framework of Universitat Autònoma de Barcelona Materials Science Ph.D. program. J.L. is a Serra Húnter Fellow and is grateful to ICREA Academia program.
Derechos:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.
Lengua:	Anglès
Documento:	Article ; recerca ; Versió publicada
Materia:	Alcohol oxidation ; Atomically dispersed metals ; Electrocatalytic oxidation ; Nickel ; 2D organic frameworks
Publicado en:	Advanced functional materials, Vol. 31, issue 51 (Dec. 2021) , art. 2106349, ISSN 1616-3028

DOI: 10.1002/adfm.202106349

8 p, 2.1 MB

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