Promoted Photocatalytic Hydrogen Evolution by Tuning the Electronic State of Copper Sites in Metal‐Organic Supramolecular Assemblies

Author:

Liu Ning1,Jiang Jialong1,Chen Zhonghang1,Wu Boyuan1,Zhang Shiqi1,Zhang Yi‐Quan2,Cheng Peng1,Shi Wei1ORCID

Affiliation:

1. Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry (MOE) Frontiers Science Center for New Organic Matter and Renewable Energy Conversion and Storage Center (RECAST) College of Chemistry Nankai University Tianjin 300071 China

2. School of Physical Science and Technology Nanjing Normal University Nanjing 210023 P. R. China

Abstract

AbstractThe electronic state in terms of charge and spin of metal sites is fundamental to govern the catalytic activity of a photocatalyst. Herein, we show that modulation of the electronic states of Cu sites, without changing the coordination environments, of two metal‐organic supramolecular assemblies based on π⋅⋅⋅π stacking can significantly improve photocatalytic activity. The use of these heterogeneous photocatalysts, without using noble metal cocatalysts, resulted in an increase of the hydrogen production rate from 522 to 3620 μmol h−1 g−1. A systematical analysis revealed that the charge density and spin density of the metal centers are efficiently modulated via the modulation of the coordination fields around active copper (II) centers by the variation of the non‐coordination groups of terminal ligands, leading to the significant enhancement of photocatalytic activity. This work provides an insight into the electronic state of active metal centers for designing high‐performance photocatalysts.

Publisher

Wiley

Subject

General Chemistry,Catalysis

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