文献类型：期刊文献

英文题名：Nitrogen-Rich Carbon Dot-Mediated n→π Electronic Transition in Carbon Nitride for Superior Photocatalytic Hydrogen Peroxide Production

作者：Guo, Huazhang[1];Zhou, Li[1];Huang, Kai[2,3];Li, Yongqiang[4];Hou, Weidong[1];Liao, Huange[1];Lian, Cheng[2,3];Yang, Siwei[4];Wu, Deli[5];Lei, Zhendong[5,6];Liu, Zheng[6];Wang, Liang[1]

机构：[1]Shanghai Univ, Inst Nanochem & Nanobiol, Sch Environm & Chem Engn, 99 Shangda Rd, Shanghai 200444, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Shanghai Inst Microsyst & Informat Technol, Chinese Acad Sci, State Key Lab Mat Integrated Circuits, Shanghai 200050, Peoples R China;[5]Tongji Univ, Coll Environm & Engn, Shanghai 200092, Peoples R China;[6]Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore

年份：2024

卷号：34

期号：38

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20241916048731);WOS:【SCI-EXPANDED(收录号:WOS:001215075400001)】；

基金：H.G. and L.Z. contributed equally to this work. The project was funded by the China Postdoctoral Science Foundation (2023T160406) and the Shanghai Pujiang Program (21PJD022). This project was also supported by the Singapore Ministry of Education AcRF Tier 2 (MOE-MOET2EP10121-0006) and AcRF Tier 1 (Shanghai Technical Service Center of Science and Engineering Computings). This work was supported by the Shanghai Technical Service Center of Science and Engineering Computing, Shanghai University.

语种：英文

外文关键词：carbon dots; carbon nitride; hydrogen peroxide production; n ->pi* electronic transition; photocatalysis

摘要：Solar-driven synthesis of hydrogen peroxide (H2O2) through photocatalysis stands out as a promising avenue for sustainable energy generation, marked by environmental friendliness and industrial feasibility. However, the inherent limitations of carbon nitride (CN) in photocatalytic H2O2 production significantly impede their performance. Herein, a novel 0D/2D carbon dots-modified CN nanosheet heterojunction (CDsMCN) is introduced, synthesized through a hydrothermal-calcination tandem strategy induced by CDs derived from melamine. This innovative technique enhances the n ->pi* electronic transition in CDsMCN, accelerating the separation efficiency of electron-hole pairs, boosting oxygen adsorption, and promoting a highly selective 2e(-) ORR. Comparative to pristine CN, CDs(10)MCN exhibited a remarkable tenfold increase in H2O2 production, reaching an impressive 1.48 mmol L-1. Furthermore, CDs(10)MCN demonstrates exceptional stability, maintaining its catalytic efficiency at the initial level over four consecutive cycles. The notable achievement of a molar selectivity of H2O2 approximate to 80% at an onset potential of 0.6 V (vs RHE) underscores its exceptional ability to produce the desired product selectively. Advanced in situ characterization together with DFT calculations revealed that the ultrathin CDs(10)MCN nanosheet heterojunction with enhanced n ->pi* electronic transition improves its optical properties, reduces bandgap, facilitates fast charge migration, and increases photocatalytic H2O2 performance, thereby serving as a promising candidate for advanced catalytic applications.