Formation of BNC Coordination to Stabilize the Exposed Active Nitrogen Atoms in g‐C3N4 for Dramatically Enhanced Photocatalytic Ammonia Synthesis Performance

Small - Tập 16 Số 13 - 2020
Weikang Wang1,2, Hongjian Zhou1, Yanyan Liu1,2, Haimin Zhang1,2, Yunxia Zhang1, Guozhong Wang1, Huijun Zhao3
1Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, Anhui, 230031 China
2Science Island Branch of Graduate School, University of Science and Technology of China, Hefei, Anhui 230026, China
3Centre for Clean Environment and Energy Griffith University Gold Coast Campus, Queensland 4222, Australia

Tóm tắt

AbstractIt is an important issue that exposed active nitrogen atoms (e.g., edge or amino N atoms) in graphitic carbon nitride (g‐C3N4) could participate in ammonia (NH3) synthesis during the photocatalytic nitrogen reduction reaction (NRR). Herein, the experimental results in this work demonstrate that the exposed active N atoms in g‐C3N4 nanosheets can indeed be hydrogenated and contribute to NH3 synthesis during the visible‐light photocatalytic NRR. However, these exposed N atoms can be firmly stabilized through forming BNC coordination by means of B‐doping in g‐C3N4 nanosheets (BCN) with a B‐doping content of 13.8 wt%. Moreover, the formed BNC coordination in g‐C3N4 not only effectively enhances the visible‐light harvesting and suppresses the recombination of photogenerated carriers in g‐C3N4, but also acts as the catalytic active site for N2 adsorption, activation, and hydrogenation. Consequently, the as‐synthesized BCN exhibits high visible‐light‐driven photocatalytic NRR activity, affording an NH3 yield rate of 313.9 µmol g−1 h−1, nearly 10 times of that for pristine g‐C3N4. This work would be helpful for designing and developing high‐efficiency metal‐free NRR catalysts for visible‐light‐driven photocatalytic NH3 synthesis.

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Tập 16 Số 13

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