Dynamic in situ Formation of Cu2O Sub‐Nanoclusters through Photoinduced pseudo‐Fehling's Reaction for Selective and Efficient Nitrate‐to‐Ammonia Photosynthesis

Author:

Li Jieyuan1ORCID,Chen Ruimin1,Wang Jielin1,Wang Kaiwen2,Zhou Ying3,Xing Mingyang4,Dong Fan1ORCID

Affiliation:

1. Research Center for Carbon-Neutral Environmental & Energy Technology Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 611731 China

2. Beijing Key Lab of Microstructure and Properties of Advanced Materials Beijing University of Technology Beijing 100124 China

3. The Center of New Energy Materials and Technology School of New Energy and Materials Southwest Petroleum University Chengdu 610500 China

4. School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China

Abstract

AbstractCopper (Cu) is evidenced to be effective for constructing advanced catalysts. In particular, Cu2O is identified to be active for general catalytic reactions. However, conflicting results regarding the true structure‐activity correlations between Cu2O‐based active sites and efficiencies are usually reported. The structure of Cu2O undergoes dynamic evolution rather than remaining stable under working conditions, in which the actual reaction cannot proceed over the prefabricated Cu2O sites. Therefore, the dynamic construction of Cu2O active sites can be developed to promote catalytic efficiency and reveal the true structure‐activity correlations. Herein, by introducing the redox pairs of Cu2+ and reducing sugar into a photocatalysis system, it is clarified that the Cu2O sub‐nanoclusters (NCs), working as novel active sites, are on‐site constructed on the substrate via a photoinduced pseudo‐Fehling's route. The realistic interfacial charge separation and transformation capacities are remarkably promoted by the dynamic Cu2O NCs under the actual catalysis condition, which achieves a milestone efficiency for nitrate‐to‐ammonia photosynthesis, including the targets of production rate (1.98±0.04 mol gCu−1 h−1), conversion ratio (94.2±0.91 %), and selectivity (98.6 %±0.55 %). The current work develops an effective strategy for integrating the active site construction into realistic reactions, providing new opportunities for Cu‐based chemistry and catalysis sciences research.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

General Chemistry,Catalysis

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