用户名: 密码: 验证码:
人工光合成材料的原子尺度精确结构调控与催化
详细信息    查看官网全文
摘要
传统能源的大量消耗已带来全球性的能源危机与环境污染,因此,人工光合成作为理想的太阳能利用与储存技术得到广泛关注。通过结构调控来加速与控制人工光合成材料固液界面的催化反应,已成为该领域研究的热点。首先,我们制备出一种新型助催化剂材料:Pt O,借助实验和理论共同发现其单向抑制氢气氧化反应的独特性质[1],进一步阐明了传统金属Pt的存在对催化产氢活性无影响,而氧化态的Ptδ+才是真正的催化活性中心[2],并证明了多种贵金属单原子在光解水产氢方面的高稳定性和高催化活性[3]。此外,通过对g-C3N4材料表面进行氢键修饰,有效提升其光解水性能[4]。合成了具有内嵌类发色团结构的橘色锗酸锌,实验和计算显示其可见光响应来源于内部Ge-Ge成键[5]。最后,通过对WO3材料表面与本体结构修饰,实现其催化产氢活性的激活,并提出一种在一般意义上设计制备高效催化剂的理念:从完全无活性的金属氧化物出发,通过原子尺度精确结构调控获得高效水分解产氢催化剂[6]。
Artificial photosynthesis has attracted intensive research efforts due to its potential for solar energy conversion.Theoretical investigation as well as the experimental design for the catalytic reaction occurred on the solid-liquid interface remain to be crucial challenges in this process.Herein,we rationally design a series of high-efficiency catalysts for hydrogen evolution in water splitting,including noble metal species(Pt O,single-atom cocatalysts,etc.),H-bonding network decorated g-C_3N_4,amorphous Zn-Ge-O as well as WO_2.9.The theoretical calculations reveal that the superior catalytic activities derive from the precise atomic structure engineering,which is capable of suppressing the undesirable back reaction and recombination of photo-generated charges as well as tailoring the unfavorable band structure or the binding energy with H atom.Therefore,these findings illustrate the significance of atomic structure engineering and should pave the way for efficient solar conversion devices.
引文
[1]Y.H.Li,J.Xing,Z.J.Chen,H.F.Wang*,P.Hu,H.J.Zhao,H.G.Yang*,Nat.Commun.,2013,4,2500.
    [2]J.Xing,H.B.Jiang,J.F.Chen,Y.H.Li,L.Wu,S.Yang,L.R.Zheng,H.F.Wang*,P.Hu,H.J.Zhao,H.G.Yang*,J.Mater.Chem.A,2013,1,15258.
    [3]J.Xing,J.F.Chen,Y.H.Li,W.T.Yuan,Y.Zhou,L.R.Zheng,H.F.Wang*,Y.Wang,H.J.Zhao,Y.Wang,H.G.Yang*,Chem.Eur.J.,2014,20,2138.
    [4]X.L.Wang,H.F.Wang,H.Zhang,H.Zhao,Y.Yao*,H.G.Yang*,J.Mater.Chem.A,2013,1,14089.
    [5]L.Qian,J.F.Chen,Y.H.Li,L.Wu,H.F.Wang,A.P.Chen,P.Hu,L.R.Zheng*,H.G.Yang*,Angew.Chem.Int.Ed.,2015,54,11467.
    [6]Y.H.Li,P.F.Liu,L.F.Pan,H.F.Wang,Z.Z.Yang,L.R.Zheng,P.Hu,H.J.Zhao,L.Gu,H.G.Yang*,Nat.Commun.,2015,6,8064.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700