Facile "Spot-Heating" Synthesis of Carbon Dots/Carbon Nitride for Solar Hydrogen Evolution Synchronously with Contaminant Decomposition

被引:188
作者
Zhang, Gong [1 ]
Ji, Qinghua [1 ]
Wu, Zhang [2 ]
Wang, Guichang [3 ,4 ]
Liu, Huijuan [1 ,2 ,5 ]
Qu, Jiuhui [1 ,5 ,6 ]
Li, Jinghong [7 ]
机构
[1] Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R China
[2] Chinese Acad Sci, Res Ctr Eco Environm Sci, State Key Lab Environm Aquat Chem, Beijing 100085, Peoples R China
[3] Nankai Univ, Coll Chem, Minist Educ, Key Lab Adv Energy Mat Chem, Tianjin 300071, Peoples R China
[4] Nankai Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300071, Peoples R China
[5] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[6] Chinese Acad Sci, Res Ctr Eco Environm Sci, Key Lab Drinking Water Sci & Technol, Beijing 100085, Peoples R China
[7] Tsinghua Univ, Dept Chem, Key Lab Bioorgan Phosphorus Chem & Chem Biol, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
carbon dots; carbon nitride; degradation; H-2; production; metal-free photocatalysts; PHOTOCATALYTIC H-2 EVOLUTION; VISIBLE-LIGHT; QUANTUM DOTS; ARTIFICIAL PHOTOSYNTHESIS; ENHANCED PHOTOCATALYSIS; WATER; HETEROJUNCTION; SURFACE; NANOSTRUCTURES; SEMICONDUCTORS;
D O I
10.1002/adfm.201706462
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The use of solar energy to produce the clean hydrogen (H-2) energy from water splitting is a promising means of renewable energy conversion. High activation barriers for O-2 generation associated with the rate-limiting steps require utilization of noble metal-based cocatalysts, which complicates the fabrication procedure and compromises the stability of the catalyst. Here, a homogenous "spot heating" approach is designed via the ultrasonic cavitation effect for evenly embedding highly crystalline carbon quantum dots (CQDs) on 2D C3N4 nanosheets. Based on density functional calculations and electrochemical experiments, the optimal introduction of CQDs into C3N4 not only extends light absorption spectrum, but also reduces effective mass of electrons (e(-)), facilitating photocarrier transport from excited sites. And, more importantly, the well-organized CQDs with superior peroxidase mimetic activity can increase catalytic H-2 production through the process of (i) 2H(2)O -> H2O2 + H-2; (ii) H2O2 -> 2 center dot OH; (iii) center dot OH + bisphenol A. Final Products, with H-2 production rate (152 mu mol g(-1) h(-1)) several times higher than that for pure C3N4. This work demonstrates an ideal platform for efficient H-2 production with synergetic organic contaminant degradation, thereby opening possibilities for coupling energy conversion with environmental remediation.
引用
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页数:8
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