纳米棒
材料科学
氮化物
氮化碳
纳米技术
光合作用
碳纤维
光电子学
化学
复合材料
图层(电子)
光催化
复合数
生物化学
催化作用
作者
Aiyun Meng,Xinyuan Ma,Da Wen,Wei Zhong,Shuang Zhou,Yaorong Su
出处
期刊:Chinese Journal of Catalysis
[China Science Publishing & Media Ltd.]
日期:2024-05-01
卷期号:60: 231-241
被引量:1
标识
DOI:10.1016/s1872-2067(24)60008-2
摘要
Graphitic carbon nitride (g-C3N4) shows great potential in photocatalytic H2O2 production. However, challenges arise from its low in-plane crystallinity and selectivity in two-electron oxygen reduction reaction (2e−-ORR), greatly limiting its H2O2 photosynthesis efficiency. Herein, we develop an ingenious strategy to simultaneously increase the in-plane crystallinity and induce the highly-selective 2e−-ORR by rationally designing barium (Ba) atom-implanted in-plane highly ordered g-C3N4 nanorods. The approach involves controllable synthesis of in-plane high crystallinity g-C3N4 nanorods with Ba implantation (BI-CN) using a BaCl2-mediated in-plane polymerization strategy. The unique Ba-N interaction induces the oriented polymerization of 3-s-triazine units to form well-arranged in-plane structures. Experimental and theoretical calculations clarify that the implanted Ba atoms function as positive charge centers, resulting in a Pauling-type O2 adsorption configuration. This minimizes O–O bond breaking energy, thus suppressing the four-electron oxygen reduction reaction (4e−-ORR) and facilitating a highly-selective 2e−-ORR pathway for efficient photocatalytic H2O2 production. Consequently, the optimized BI-CN3 photocatalyst exhibits an outstanding H2O2 production rate of as high as 353 μmol L−1 h−1, surpassing the pristine g-C3N4 by 6.1 times. This study concurrently optimizes the in-plane crystallinity and O2 adsorption sites of g-C3N4 photocatalysts for highly-selective H2O2 production, providing innovative insights for designing efficient photocatalysts with diverse applications.
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