新型直接Z-型光催化材料的设计制备与应用基础研究

项目来源

国家自然科学基金(NSFC)

项目主持人

余家国

项目受资助机构

武汉理工大学

项目编号

U1705251

立项年度

2017

立项时间

未公开

项目级别

国家级

研究期限

未知 / 未知

受资助金额

204.00万元

学科

联合基金领域-新材料与先进制造领域

学科代码

L-L04

基金类别

联合基金项目-重点支持项目-促进海峡两岸科技合作联合基金

关键词

直接Z-型 ; 产氢 ; CO2还原 ; 太阳燃料 ; 光催化材料 ; Direct Z-scheme ; photocatalytic materials ; hydrogen production ; CO2 reduction ; solar fuels

参与者

李朝晖;吴嘉文;傅俊伟;朱必成;夏鹏飞;蔡静宇;邓筱羽;王冰清;廖佑德

参与机构

福州大学;台湾大学

项目标书摘要:本项目以实现直接Z-型光催化材料高效分解水产氢和CO2还原制备太阳燃料为目标,解决传统单一光催化材料光生电子和空穴容易复合,以及它们的还原或氧化能力不足等关键科学问题。重点研究直接Z-型光催化产氢和CO2还原材料设计与制备方法、表面界面微结构调控、光生载流子转移分离与光催化机理,通过两种半导体耦合形成直接Z-型异质结,提高光催化材料的产氢和CO2还原效率,其产氢和CO2还原效率达到国际先进水平。阐明直接Z-型光催化材料的化学组成、制备方法、形貌、表面结构等对光催化产氢和CO2还原性能的影响规律,揭示直接Z-型光催化材料的构—效关系,建立新型直接Z-型光催化产氢和CO2还原材料的设计思想与制备方法。在高效直接Z-型光催化材料研究领域取得具有国际水准的原创性研究成果,建立一支交叉融合的多学科研究队伍和研究平台,为增强我国在光催化产氢和CO2还原材料领域的国际竞争力做出实质性贡献。

Application Abstract: The objective of this project is the fabrication of direct Z-scheme photocatalytic materials used for the preparation of solar fuels by highly efficient photocatalytic hydrogen production from water-splitting and CO2-reduction,and for solving the high recombination rate of photogenerated electron-hole pairs and their lower reduction and oxidation ability in single photocatalyst.The main research work includes design and fabrication of direct Z-scheme photocatalytic H2-production and CO2-reduction materials,microstructure control of surface and interface,transfer and separation of photogenerated charge carriers,and the mechanism of photocatalytic reactions.The photocatalytic H2-production and CO2-reduction efficiency will be significantly improved by constructing direct Z-scheme heterojunction between two semiconductors.The effects of chemical composition,preparation method,morphology,surface structure etc.on photocatalytic H2-production and CO2-reduction performance of direct Z-scheme photocatalyst will be carefully investigated and discussed.The composition-structure-performance intrinsic relationship and synergistic effect between two semiconductor photocatalysts will be established.New design idea and method for the preparation of direct Z-scheme photocatalyst used for hydrogen production and CO2 reduction will be developed and proposed.This investigation will also provide new insight into the design and fabrication of direct Z-scheme photocatalysts used for hydrogen production and CO2 reduction.

项目受资助省

湖北省

项目结题报告(全文)

项目以实现直接Z-型光催化材料高效分解水产氢和CO2还原制备太阳燃料为目标,解决传统单一光催化材料光生载流子容易复合,以及还原或氧化能力不足等关键科学问题。研究了直接Z-型和S-型光催化产氢和CO2还原材料设计与制备方法、表面界面微结构调控、光生载流子转移分离与光催化机理。通过两种半导体耦合形成直接Z-型和S-型异质结,提高了光催化材料的产氢和CO2还原效率,其产氢和CO2还原效率达到国际先进水平。阐明了直接Z-型和S-型光催化材料的化学组成、制备方法、形貌、表面结构等对光催化产氢和CO2还原性能的影响规律,揭示了直接Z-型和S-型光催化材料的构—效关系,建立了新型直接Z-型和S-型光催化产氢和CO2还原材料的设计思想与制备方法。为了克服传统Z-型光催化和全固态Z-型光催化的缺陷,项目期间提出了梯形(Step-scheme or S-scheme)异质结光催化的新概念。多篇研究论文发表在多种国际刊物上,如:Nature Commun.、Adv.Mater.、Chem、Angew.Chem.Int.Ed.、Joule、Chem.Rev.等,论文被SCI 收录172篇,论文中有高被引论文52篇,热点论文7篇,被SCI他人引文12874次。项目期间毕业了19位博士和39位硕士,出站博士后6人。研究成果获得湖北省自然科学一等奖1项,有4人入选科睿唯安全球高被引科学家名单,1人获得基金委优青资助。出版英文学术专著2部和中文学术专著1部,分别是:Surface Science of Photocatalysis,Elsevier,2020;Semiconductor Solar Photocatalysts:Fundamentals and Applications,Wiley,2021;和新型太阳燃料光催化材料,武汉理工大学出版社,2018。获授权发明专利13项。主办国际会议6次,在国际国内会议做大会和邀请报告38次。项目负责人余家国2020年入选欧洲人文与自然科学院和欧洲科学院两院外籍院士;2020年获得第二届全国创新争先奖,全国创新争先奖每3年评选表彰一次,每次不超过300人。获得第35届花拉子米国际奖(35th Khwarizmi International Award)。

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    • CO2 reduction; nitrogen-doped graphene structure; nitrogen-dopedgraphene based photocatalysis; nitrogen-doped graphene synthesis

    Solving energy and environmental problems through solar-driven photocatalysis is an attractive and challenging topic. Hence, various types of photocatalysts have been developed successively to address the demands of photocatalysis. Graphene-based materials have elicited considerable attention since the discovery of graphene. As a derivative of graphene, nitrogen-doped graphene (NG) particularly stands out. Nitrogen atoms can break the undifferentiated structure of graphene and open the bandgap while endowing graphene with an uneven electron density distribution. Therefore, NG retains nearly all the advantages of original graphene and is equipped with several novel properties, ensuring infinite possibilities for NG-based photocatalysis. This review introduces the atomic and band structures of NG, summarizes in situ and ex situ synthesis methods, highlights the mechanism and advantages of NG in photocatalysis, and outlines its applications in different photocatalysis directions (primarily hydrogen production, CO2 reduction, pollutant degradation, and as photoactive ingredient). Lastly, the central challenges and possible improvements of NG-based photocatalysis in the future are presented. This study is expected to learn from the past and achieve progress toward the future for NG-based photocatalysis.

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  • 7. Type: Conference Papers and Presentations Status: Published Year Published: 2013 Citation: Manzo, R.D., Gomez-Camacho, R. Martinez, L., Aguilera, A. Implementation of a Community-Based, Multi-Year, Multifaceted Program in Mexican-Origin, Rural Communities in Californias Central Valley. Interdisciplinary Graduate and Professional Symposium. April 5, 2013. University of California, Davis.

  • 8.Challenges for photocatalytic overall water splitting

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    • TIO2

    The hydrogen economy is a sunrise industry, which is considered the ultimate solution to power the future society. Photocatalytic overall water splitting is projected as a potential technology for H2 production. However, its performance is still far from meeting the criteria for large-scale production. This paper argues that photocatalytic overall water splitting is theoretically and practically hard to achieve. The limiting factors, including unfavorable thermodynamics, slow kinetics, dissolved oxygen, and rapid backward reaction, are discussed. This paper is expected to give readers a better understanding of the photocatalytic overall water splitting and analyze the associated challenges in every subtle aspect.

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    With the demanding detection of unique toxic gas, semiconductor gas sensors have attracted tremendous attention due to their intriguing features, such as, high sensitivity, online detection, portability, ease of use, and low cost. Triethylamine, a typical gas of volatile organic compounds, is an important raw material for industrial development, but it is also a hazard to human health. This review presents a concise compilation of the advances in triethylamine detection based on chemiresistive sensors. Specifically, the testing system and sensing parameters are described in detail. Besides, the sensing mechanism with characterizing tactics is analyzed. The research status based on various chemiresistive sensors is also surveyed. Finally, the conclusion and challenges, as well as some perspectives toward this area, are presented.

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  • 10.g-C3N4-Based 2D/2D Composite Heterojunction Photocatalyst

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    • charge separation; graphitic carbon nitride; photocatalysis; S-scheme;2D/2D heterojunction;GRAPHITIC CARBON NITRIDE; Z-SCHEME HETEROJUNCTION; CHARGE-TRANSFERNANOCHANNELS; ENERGY-BAND STRUCTURE; IN-SITU CONSTRUCTION;VISIBLE-LIGHT; HIGH-PERFORMANCE; HYDROGEN EVOLUTION; NANOSHEETHETEROJUNCTIONS; HYBRID HETEROJUNCTION

    Employing semiconductor photocatalysis to transform solar energy into chemical energy provides a practicable strategy for the alleviation of energy and environmental crisis. Graphitic carbon nitride (g-C3N4) is a popular 2D photocatalyst with numerous advantages, such as visible light response, low cost, and high stability. However, single g-C3N4 photocatalyst displays poor performance due to fast recombination of photogenerated electrons and holes. To improve this limitation, many research works have focused on the construction of g-C3N4-based 2D/2D heterojunction photocatalysts by hybridizing g-C3N4 with other 2D materials. The intimate face-to-face contact in 2D/2D heterojunction offers large contact area and plentiful channels for the migration and separation of photogenerated charge carriers. Furthermore, 2D/2D heterojunction inherits the strengths of 2D structure, including high specific surface area, abundant adsorption sites and active sites. Herein, the preparation, mechanism, and application of g-C3N4-based 2D/2D heterojunction photocatalysts are reviewed. Three common preparation methods are summarized, including solid phase reaction, in situ growth, and electrostatic self-assembly. Various photocatalytic mechanisms are discussed, including traditional type-II, Z-scheme and S-scheme mechanisms. A series of applications in energy and environment fields are illustrated. Finally, future directions for the development of g-C3N4-based 2D/2D heterojunction photocatalysts are proposed.

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