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Oxygen-incorporated carbon nitride porous nanosheets for highly efficient photoelectrocatalytic CO2 reduction to formate

WANG Hong-zhi ZHAO Yue-zhu YANG Zhong-xue BI Xin-ze WANG Zhao-liang WU Ming-bo

王虹智, 赵悦竹, 杨中学, 毕鑫泽, 王照亮, 吴明铂. 氧掺杂氮化碳多孔纳米片高效光电催化二氧化碳还原制甲酸. 新型炭材料. doi: 110.1016/S1872-5805(22)60619-X
引用本文: 王虹智, 赵悦竹, 杨中学, 毕鑫泽, 王照亮, 吴明铂. 氧掺杂氮化碳多孔纳米片高效光电催化二氧化碳还原制甲酸. 新型炭材料. doi: 110.1016/S1872-5805(22)60619-X
WANG Hong-zhi, ZHAO Yue-zhu, YANG Zhong-xue, BI Xin-ze, WANG Zhao-liang, WU Ming-bo. Oxygen-incorporated carbon nitride porous nanosheets for highly efficient photoelectrocatalytic CO2 reduction to formate. New Carbon Mater.. doi: 110.1016/S1872-5805(22)60619-X
Citation: WANG Hong-zhi, ZHAO Yue-zhu, YANG Zhong-xue, BI Xin-ze, WANG Zhao-liang, WU Ming-bo. Oxygen-incorporated carbon nitride porous nanosheets for highly efficient photoelectrocatalytic CO2 reduction to formate. New Carbon Mater.. doi: 110.1016/S1872-5805(22)60619-X

氧掺杂氮化碳多孔纳米片高效光电催化二氧化碳还原制甲酸

doi: 110.1016/S1872-5805(22)60619-X
基金项目: 国家自然科学基金(52072409);山东省自然科学基金(ZR2021QE062);山东省科技创新重大专项(2020CXGC010402);青岛市博士后应用研究项目(qdyy20200063);泰山学者项目(ts201712020)
详细信息
    通讯作者:

    王照亮,博士,教授. E-mail:wzhaoliang@upc.edu.cn

    吴明铂,博士,教授. E-mail:wumb@upc.edu.cn

Oxygen-incorporated carbon nitride porous nanosheets for highly efficient photoelectrocatalytic CO2 reduction to formate

Funds: This work was financially supported by the National Natural Science Foundation of China (52072409), Natural Science Foundation of Shandong Province (ZR2021QE062), Major Scientific and Technological Innovation Project of Shandong Province (2020CXGC010402), Qingdao postdoctoral applied research project (qdyy20200063), and Taishan Scholar Project (No. ts201712020)
More Information
  • 摘要: 利用二氧化碳作为可再生的碳源来生产高价值的燃料和化学品最近引起了全球的关注。在现有的CO2转化方法中,光电催化CO2还原反应(CO2RR)是最有效和最有前景的选择之一,它可以在模拟太阳光照和低过电位条件下实现。本文成功地合成了含氧氮化碳(CN)多孔纳米片作为光电阳极,Bi2CuO4作为光电阴极,实现光电催化CO2还原生成甲酸盐。通过改变氧源,成功地调节了CN的导电性能和光电响应性能。前驱体中氧的电负性更强,因此可以提高CN的导电性能。而焙烧气氛中的氧却通过改变能带结构对光电响应性能产生了不利影响。在最优条件下,CN的光电流密度高达587 μA cm−2,CO2还原成甲酸的活性为273.56 µmol cm−2 h−1(约为常规样品的19倍)。此外,CN样品在24小时恒定的光电流下表现出良好的稳定性。本研究为实现高效的光电催化CO2还原成甲酸提供了一种新的途径,并可通过不同阴极催化剂的偶联,扩展到其他PEC反应。
  • Figure  1.  (a) Schematic of the synthesis derived from melamine or/and urea. TEM images of CN1 (b), CN2 (c), CN3 (d) and CN4 (e), inset digital photographs show CN nanosheets solution, respectively.

    Figure  2.  X-ray diffraction patterns (a), FT-IR spectra (b), EPR spectra (c), and steady-state PL spectra (d) of CN samples.

    Figure  3.  (a) LSV curves. (b) LSV curves of CN1 under dark (full line) and AM 1.5G illumination (dotted line). (c) Transient amperometric I–t curves at −0.9 V vs. RHE under AM 1.5G illumination. (d) Photocurrent stability of CN1 photoanode under AM 1.5G illumination.

    Figure  4.  (a) Schematic illustration of AM 1.5G light induced electron/hole separation and transfer process during PEC CO2RR in CN photoanode. (b) The PEC performance of CN samples toward CO2 reduction to formate.

    Figure  5.  UV–vis absorption spectra (a), Tauc plots (b), the band alignment (c) and XPS spectra of O1s (d) for CN samples.

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  • 收稿日期:  2022-01-01
  • 网络出版日期:  2022-06-13

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