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One-photo excitation pathway in 2D in-plane heterostructures for effective visible-light-driven photocatalytic degradation
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作者 Mengchi Liu Yiwen Cheng +4 位作者 Yuee Xie yingcong wei Jinhui Xing Yuanping Chen Jing Xu 《Journal of Semiconductors》 EI CAS CSCD 2023年第5期42-52,共11页
Broad-spectrum absorption and highly effective charge-carrier separation are two essential requirements to improve the photocatalytic performance of semiconductor-based photocatalysts.In this work,a fascinating one-ph... Broad-spectrum absorption and highly effective charge-carrier separation are two essential requirements to improve the photocatalytic performance of semiconductor-based photocatalysts.In this work,a fascinating one-photon system is reported by rationally fabricating 2D in-plane Bi_(2)O_(3)/BiOCl(i-Cl)heterostructures for efficient photocatalytic degradation of RhB and TC.Systematic investigations revealed that the matched band structure generated an internal electric field and a chemical bond connection between the Bi_(2)O_(3)and BiOCl in the Bi_(2)O_(3)/BiOCl composite that could effectively improve the utilization ratio of visible light and the separation effectivity of photo-generated carriers in space.The formed interactions at the 2D in-plane heterojunction interface induced the one-photon excitation pathway which has been confirmed by the experiment and DFT calculations.As a result,the i-Cl samples showed significantly enhanced photocatalytic efficiency towards the degradation of RhB and TC(RhB:0.106 min^(-1);TC:0.048 min^(-1))under visible light.The degradation activities of RhB and TC for i-Cl were 265.08 and 4.08times that of pure BiOCl,as well as 9.27 and 2.14 times that of mechanistically mixed Bi_(2)O_(3)/BiOCl samples,respectively.This work provides a logical strategy to construct other 2D in-plane heterojunctions with a one-photon excitation pathway with enhanced performance. 展开更多
关键词 photocatalysis CAU-17 Bismuth oxyhalides one-photon excitation pathway 2D in-plane heterojunction
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非贵金属等离子共振增强MoO_(3-x)基S型异质结光催化苯甲醇氧化同步产氢和苯甲醛
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作者 魏英聪 张琪琪 +7 位作者 周颖 马雄风 王乐乐 王严杰 洒荣建 龙金林 付贤智 员汝胜 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第10期2665-2677,共13页
氢燃料具有无污染与高质量能量密度的特点使其成为一种重要的清洁能源.通过半导体光催化过程将太阳能转化为氢能,是应对能源与环境问题的理想方案之一.在传统光催化产氢过程中,光生电子可将质子还原生成氢气,而同步产生的光生空穴一般... 氢燃料具有无污染与高质量能量密度的特点使其成为一种重要的清洁能源.通过半导体光催化过程将太阳能转化为氢能,是应对能源与环境问题的理想方案之一.在传统光催化产氢过程中,光生电子可将质子还原生成氢气,而同步产生的光生空穴一般被牺牲剂消耗.虽然反应体系中牺牲剂的添加可以有效提升产氢速率,但是空穴的氧化能力没有得到有效利用.同时,昂贵牺牲剂的使用极大制约了光催化制氢半反应的经济效益和应用前景.通过有机物无氧脱氢反应,同步生成氢气和高附加值有机化合物,不仅实现了电子和空穴的同步利用,而且提升了太阳能的转化效率.尽管这类双功能催化剂近年来已有少量报道,但仍存在光吸收范围窄(紫外-可见光)、掺杂贵金属或载流子分离效率低等问题.因此,开发廉价、高活性、全光谱吸收的催化材料及体系仍是重要且极具挑战性的任务.本文报道了一种非贵金属(MoO_(3-x))等离子共振增强的全光谱响应(200–1400 nm)Zn_(0.1)Cd_(0.9)S/MoO_(3-x) S型异质结光催化剂.以乳酸为牺牲剂时,该催化剂可实现高效光解水产氢,其产氢速率高达149.2 mmol·g^(–1)·h^(–1),是纯Zn_(0.1)Cd_(0.9)S体系的6倍.此外,当以苯甲醇同时充当电子受体和给体时,可见光(420–780 nm)和近红外光(780–1050 nm)激发均可驱动苯甲醇无氧脱氢,生成苯甲醛和氢气,从而同步有效利用光生电子与空穴.该体系较高的催化效率主要由于:Zn_(0.1)Cd_(0.9)S纳米棒和MoO_(3-x)纳米片之间的界面紧密接触以及内建电场对光生电子转移的动力学促进;S型异质结的构建有效提升了载流子分离效率,同时提高了光生载流子的氧化-还原能力;MoO_(3-x)纳米片的LSPR效应使得Zn_(0.1)Cd_(0.9)S/MoO_(3-x)复合材料具备了包含紫外-可见-近红外光区域的宽光谱吸收范围.综上,本文系统研究了不同激发能量下产氢过程的反应机理,为理性设计双功能光催化氧化-还原反应体系,实现光催化产氢与精细化学品的同步合成提供了借鉴. 展开更多
关键词 Zn_(0.1)Cd_(0.9)S/MoO_(3-x)S型异质结 局域表面等离子体共振 苯甲醇氧化 产氢 全光谱响应
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