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Nitriding Nickel-Based Cocatalyst: A Strategy To Maneuver Hydrogen Evolution Capacity for Enhanced Photocatalysis

  • Li Li
    Li Li
    School of the Environment and Safety Engineering, Institute for Energy Research,  Analysis and Testing Center, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Li Li
  • Jianjian Yi
    Jianjian Yi
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Jianjian Yi
  • Xingwang Zhu
    Xingwang Zhu
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Xingwang Zhu
  • Min Zhou
    Min Zhou
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Min Zhou
  • Sai Zhang
    Sai Zhang
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Sai Zhang
  • Xiaojie She
    Xiaojie She
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Xiaojie She
  • Zhigang Chen*
    Zhigang Chen
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    *E-mail: [email protected] (Z.C.).
    More by Zhigang Chen
  • Hua-Ming Li
    Hua-Ming Li
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    More by Hua-Ming Li
  • , and 
  • Hui Xu*
    Hui Xu
    School of the Environment and Safety Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, P. R. China
    *E-mail: [email protected] (H.X.).
    More by Hui Xu
Cite this: ACS Sustainable Chem. Eng. 2020, 8, 2, 884–892
Publication Date (Web):December 12, 2019
https://doi.org/10.1021/acssuschemeng.9b05248
Copyright © 2019 American Chemical Society
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Abstract

Seeking earth-abundant cocatalysts for boosting the photocatalytic performance of the host semiconductor is of great significance. Here, enlightened by the structural optimization strategy concerning nitridation treatment on various advanced materials, the nickel nitride (Ni3N) nanocrystals were prepared. To understand the catalytic behavior and structure–performance correlation, the Ni3N was loaded on the surface of two-dimensional carbon nitride (2D-C3N4), forming a typical 0D–2D architecture. The well-assembled 0D–2D nanohybrids ultimately achieved the high efficiency catalysis of H2 evolution rate reaching ∼1347.8 μmol/g/h (external quantum efficiency = 2.3% at 420 nm), ranking at the forefront among the 2D-C3N4 supported Ni-based cocatalysts and noble metals (e.g., Au, Ag, Pd). Combined with theoretical calculation and spectrum characterization, we propose that the enhanced hydrogen evolution performance can be ascribed to the improved charge transport ability and optimized H* adsorption/desorption capacity. Ultimately, the balance between the surface of Ni3N and protons is conducive to the boosted hydrogen evolution reaction performance. This work demonstrates the potential of transition-metal nitrides to establish high-efficiency photocatalytic cell without using noble metals for water splitting.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.9b05248.

  • Experimental details, SEM and TEM images of Ni3N, UV–vis diffuse reflectance spectra of Ni3N, 2D-C3N4, and Ni3N/2D-C3N4 composite, photocatalytic HER performance of 2D-C3N4, 2D-C3N4 after NH3 treatment and optimal Ni3N/2D-C3N4 composite, N2 absorption–desorption isotherms of 2D-C3N4 and Ni3N/2D-C3N4 composite, XRD patterns and FT-IR spectra of 2D-C3N4 before and after NH3 treatment, EDX spectra for the optimal Ni3N/2D-C3N4 composite, FT-IR spectra of bare 2D-C3N4 and 10% Ni3N/2D-C3N4, XPS survey spectra, C 1s XPS spectra of the 10% Ni3N/2D C3N4 and Ni3N, ESR spectra of DMPO-O2•– and OH adducts under and without the visible-light irradiation of Ni3N, schematic of catalytic hydrogen evolution process, photocatalytic performance at different reaction conditions over different catalysts, calculation process of EQE and comparison of and table for performance comparison with previous reports (PDF)

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