摘要
水滑石(LDHs)具有独特的层状结构、可调的组成、可控的粒径大小和形貌、简单的合成方法、易于放大生产制备等特点,使其具有丰富的可调控性;进一步经过拓扑转变,可制备得到复合金属氧化物、负载型金属催化剂,为设计具有能带结构适宜、表界面结构丰富的绿色、高效纳米催化剂提供了广阔的平台.针对温和条件下H-O,C=O,N≡N,C-C键光驱动催化活化,本文围绕"水滑石多尺度结构精准调控及催化过程强化"的主题,通过对水滑石微观精细结构、介观异质界面结构、高分散催化剂分散特性等方面进行精准调控,实现了水滑石基催化剂在光驱动分解H_2O,还原CO_2, CO加氢制高碳烃、合成氨以及降解环境污染物等反应的强化;揭示了基于能带、缺陷、界面可控的水滑石基材料制备-结构-光驱动催化性能之间的关系,从而为实现太阳能高效转化提供思路.
Due to the high photocatalytic efficiency in activating chemical bonding under mild reaction conditions,photocatalysis has been acted as a green and promising technology.However,how to improve the quantum efficiency and solar energy utilization to further enhance the photocatalytic performance remains a challenge,and it is highly desirable to rational synthesize photocatalyst with suitable energy band structure,and efficient active sites. Layered double hydroxides (LDHs)is a kind of two-dimensional materials,with molecular formula [M1-x^2+Mx^3+(OH)2]^x+ [Ax/n]^n-·mH2O.The layered structure of LDHs is similar to brucite Mg(OH)2,which is connected by the octahedral MO6 sites.The substitution of divalent metal cations (M^2+)with trivalent metal cations (M^3+)makes the layers positively charged,in which M^2+,M^3+can be as one or more of the elements such as Mg,Al,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Ga, In,etc.M^2+,M^3+ions alternately arrange in the main layers at a high atomic level to form the planar structure (a,b axis direction),and the alternation of the positively charged layers and the negatively charged anionic layers (c axis direction) constitute the three-dimensional structure of LDHs.There are many unique structural characteristic of LDHs,such as the high dispersion of the metal elements in the layers,the controllable particle size and thickness,topological transformation and so on.The above properties have provide LDH as photocatalysts as the followings reason.Firstly,the metal elements of LDHs are arranged in an alternating order at the atomic level with flexible compositions (such as Fe,Co,Ni,Ti,etc.), and can be directly used as photocatalysts due to the tunable band gap.Secondly,the topological transformation property can turn LDH materials into heterogeneous mixed metal oxides or highly supported metal-containing catalysts,which are not easily agglomerated even under reaction condition.Thirdly,based on the tunable particle size and thickness of LDHs, it is possible to adjust the morphology of LDHs into nanosc
作者
许艳旗
谭玲
王泽林
郝晓杰
王纪康
赵宇飞
宋宇飞
Yanqi Xu;Ling Tan;Zelin Wang;Xiaojie Hao;Jikang Wang;Yufei Zhao;Yu-Fei Song(State Key Laboratory of Chemical Resource Engineering,Beijing University of Chemical Technology,Beijing 100029,China;Beijing Advanced Innovation Center for Soft Matter Science and Engineering,Beijing 100029,China)
出处
《科学通报》
EI
CAS
CSCD
北大核心
2018年第34期3598-3611,共14页
Chinese Science Bulletin
基金
国家重点研发计划(2017YFB0307303)
国家重点基础研究发展计划(2014CB932104)
国家自然科学基金(U1707603,21625101,21521005,U1507102)
北京市自然科学基金(2182047)
中央高校基金(ZY1709)资助.
关键词
水滑石
多尺度结构调控
缺陷
界面
光催化
光热催化
layered double hydroxides
multiscale structural regulation
defect
interface
photocatalysis
photothermal catalysis
