Suchun Li

Harvard University

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Weifeng Yao

Shanghai University of Electric Power

Jie Sun

Shaanxi Normal University

Qunjie Xu

Shanghai University of Electric Power

Qi Zhao

University of Science and Technology Liaoning

Cunping Huang

Federal Aviation Administration

Qiang Wu

University of Science and Technology of China

Tao Zeng

Jingdezhen Ceramic Institute

Wei Chen

National University of Singapore

Wei Chen

Brookhaven National Laboratory

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Shanghai University of Electric Power

Shanghai Institute of Pollution Control and Ecological Security

University of Central Florida

China Academy of Engineering Physics

Tongji University

Chinese Academy of Sciences

Zhejiang Provincial People's Hospital

Hangzhou Medical College

Shanghai University of Engineering Science

University of Sydney

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Single Nickel Atoms Anchored on Nitrogen-Doped Graphene as a Highly Active Cocatalyst for Photocatalytic H₂ Evolution

ACS Catalysis (2018)

Qi Zhao Jie Sun Suchun Li Cunping Huang Weifeng Yao

Earth-abundant nickel is a typical non-noble-metal cocatalyst used for photocatalytic hydrogen evolution (PHE). Ni nanoparticles, however, tend to aggregate during the hydrogen production process, significantly lowering their PHE activity. To avoid aggregation, we used single atom form Ni and anchored them on vacancies in nitrogen-doped graphene (Ni-NG) as a cocatalyst for PHE. We demonstrated that Ni-NG is a robust and highly active cocatalyst for PHE from water. With only 0.0013 wt % of Ni loading, the PHE activity of composite Ni-NG/CdS photocatalyst improves by 3.4 times compared to that of NG/CdS, and it does not decay even after 10 rounds of 5-hour running. The quantum efficiency of Ni-NG/CdS for PHE reaches 48.2% at 420 nm, one of the highest efficiencies for non-noble-metal-based cocatalysts reported in the literature. Photoluminescence spectral analyses and electrochemical examinations indicated that Ni-NG coupled to CdS serves not only as an electron storage medium to suppress electron–hole recombination but also as an active catalyst for proton reduction reaction. Density functional theory calculations show that the high activity of Ni-NG/CdS composite results from the single Ni atoms trapped in NG vacancies, which significantly reduces the activation energy barrier of the hydrogen evolution reaction. This research may be valuable for developing robust and highly active noble metal free cocatalysts for solar hydrogen production.

Noble metal

10.1021/acscatal.8b03737

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Atomically confined calcium in nitrogen-doped graphene as an efficient heterogeneous catalyst for hydrogen evolution

iScience (2021)

Jie Sun Suchun Li Qi Zhao Cunping Huang Qiang Wu

Calcium is one of the most abundant and cheapest elements on earth. However, due to the lack of d-orbitals for chemical adsorption, it is generally considered as a stoichiometric reagent with no catalytic activities in heterogeneous catalysis. In this research, we have revealed that atomically confined Ca in nitrogen-doped graphene (Ca1-NG) can be an effective heterogeneous catalyst to boost both electrocatalytic and photocatalytic hydrogen evolution reactions (HER). Ca single atoms anchored in NG can efficiently enhance the HER performance due to the improvement of the interfacial charge transfer rate and suppression of the photo-generated charge recombination. Density functional theory calculations show that the high catalytic activity of Ca1-NG results from the Ca single atoms in NG, which leads to multiple H adsorption configurations with favorable ΔGH∗ values for HER. This research can be valuable for the designing of environmentally friendly, economical and efficient catalysts for renewable hydrogen production.

10.1016/j.isci.2021.102728

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Citations (22)