Self‐Adaptive Electronic Structure of Amphoteric Conjugated Ligand‐Modified 3 d Metal−C3N4 Smart Electrocatalyst by pH Self‐Response Realizing Electrocatalytic Self‐Adjustment

Author:

Zhang Beiyi1,Li Junqi1ORCID,Song Qianqian2,Pang Lingyan1,Hao Xiaodong3,Liu Junli1,Liu Xiaoxu1,Liu Hui1

Affiliation:

1. School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic Materials Shaanxi University of Science and Technology Xi'an 710021 P. R. China

2. College of Materials Science and Engineering State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Donghua University Shanghai 201620 P. R. China

3. Materials Institute of Atomic and Molecular Science Shaanxi University of Science and Technology Xi'an 710021 P. R. China

Abstract

AbstractConstructing pH‐responsive smart material provides a new opportunity to address the problem that traditional electrocatalysts cannot achieve both alkaline oxygen evolution reaction (OER) and acidic hydrogen evolution reaction (HER) activities. In this study, amphoteric conjugated ligand (2‐aminoterephthalic acid, BDC‐NH2)‐modified 3d metal‐anchored graphitic carbon nitride (3d metal−C3N4) smart electrocatalysts are constructed, and self‐adaptation of the electronic structure is realized by self‐response to pH stimulation, which results in self‐adjustment of alkaline OER and acidic HER. Specifically, the amino and carboxyl functional groups in BDC‐NH2 undergo protonation and deprotonation respectively under different pH stimulation to adapt to environmental changes. Through DFT calculations, the increase or decrease of electron delocalization range brought by the self‐response characteristic is found to lead to redistribution of the Bader charge around the modified active sites. The OER and HER activities are greatly promoted roughly 4.8 and 8.5 times over Co−C3N4 after BDC−NH2‐induced self‐adaptive processes under different environments, arising from the reduced energy barrier of O* to OOH* and ΔGH*. Impressively, the proposed BDC‐NH2‐induced smart regulation strategy is applicable to a series of 3d metal anchors for C3N4, including Co, Ni and Fe, providing a general structural upgrading method for constructing smart electrocatalytic systems.

Funder

National Natural Science Foundation of China

Education Department of Shaanxi Province

Publisher

Wiley

Subject

General Energy,General Materials Science,General Chemical Engineering,Environmental Chemistry

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