金纳米粒子的尺寸以及金-二氧化钛相互作用对表面等离激元光催化产氧的影响

引用本文: 王升扬, 曾斌, 李灿. 金纳米粒子的尺寸以及金-二氧化钛相互作用对表面等离激元光催化产氧的影响[J]. 催化学报, 2018, 39(7): 1219-1227. doi: 10.1016/S1872-2067(18)63094-3 shu

Citation: Shengyang Wang, Bin Zeng, Can Li. Effects of Au nanoparticle size and metal-support interaction on plasmon-induced photocatalytic water oxidation[J]. Chinese Journal of Catalysis, 2018, 39(7): 1219-1227. doi: 10.1016/S1872-2067(18)63094-3 shu

金纳米粒子的尺寸以及金-二氧化钛相互作用对表面等离激元光催化产氧的影响

a 中国科学院大连化学物理研究所, 催化基础国家重点实验室, 洁净能源国家实验室(筹), 能源材料化学协同创新中心, 辽宁大连 116023;
b 中国科学院大学, 北京 100049
基金项目:
国家自然科学基金（21633010）；国家重点基础研究发展计划（973计划，2014CB239400）；中国科学院战略先导专项（XDB01020300）.

摘要: 表面等离激元共振效应具有独特的光-物质相互作用的性质，因而近年来被广泛的应用到太阳能转化科学领域.通过调变金属的性质（例如组分、尺寸、形貌等）可以方便地在整个太阳能光谱范围内调节其等离子共振吸收性质，从而有效地增加光催化剂的捕光效率.尽管如此，等离激元光催化目前的能量转化效率仍处于很低的水平，主要是由于光催化剂中的电荷分离以及利用效率很低.理论上可以通过控制优化金属纳米粒子的尺寸以及金属-半导体的相互作用来促进电荷分离及利用效率，从而提高光催化剂的活性.然而，关于金属纳米粒子的尺寸以及金属-半导体的相互作用在表面等离激元光催化剂中的具体作用还亟待详细研究.本文以金/二氧化钛作为典型的表面等离激元光催化剂，通过简便的焙烧后处理可同时实现金粒子尺寸和金-氧化钛界面相互作用的调控.我们发现，催化剂的可见光产氧活性随着焙烧温度呈现火山型关系，其中600℃处理的样品表现出最高的活性，在560 nm出的表观量子效率为0.3%，接近甚至超过文献报道的同类结果.随后通过X射线衍射、扫描电镜、光电子能谱、紫外可见光谱等表征手段系统地研究了煅烧温度对于金粒子尺寸和金-氧化钛相互作用的影响.从结果表明，通过不同温度焙烧并未改变二氧化钛自身的性质，且随着温度的升高，金尺寸在600℃之前变化较小，随后突然快速长大.在排除了不同样品的吸光性能的差异后发现，产氧活性随着Au尺寸长大而减少.从光电子能谱的结果发现，金-二氧化钛的界面相互作用随焙烧温度升高而逐步增强.进一步地，通过界面周长的归一化活性得出界面相互作用与产氧活性呈现近似线性关系.最后，通过对光沉积Au样品进行不同温度的煅烧发现大尺寸Au的粒径不随煅烧温度变化，而此时的产氧活性却随焙烧温度增加而增加，这进一步验证了界面相互作用对光催化水氧化的促进作用.综合以上结果可知，最终的等离激元诱导的可见光产氧活性是由尺寸与界面相互作用共同影响的结果，尺寸和界面相互作用的变化会共同影响热电子转移效率和表面反应效率，从而改变整体的光催化产氧效率.

关键词:

English

Effects of Au nanoparticle size and metal-support interaction on plasmon-induced photocatalytic water oxidation

a State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, and the Collaborative Innovation Center of Chemistry for Energy Mate-rials (iChEM), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China
Received Date: 27 December 2017
Revised Date: 29 April 2018
Fund Project:
This work was supported by the National Natural Science Foundation of China (21633010), the National Basic Research Program of China (973 pro-gram, 2014CB239400), and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB01020300).

Abstract: Plasmonic photocatalysis with tunable light absorption has aroused significant attention in so-lar-to-chemical energy conversion. However, the energy conversion efficiency of plasmonic photo-catalysts is impeded by ineffective charge separation and the lack of highly active sites for redox reactions. In this work, the Au nanoparticle size and Au-TiO₂ interaction of the Au/TiO₂ plasmonic photocatalyst were adjusted simultaneously using a post-calcination treatment. The visi-ble-light-induced water oxidation activity exhibited a volcano-like relationship with the calcination temperature; the treated photocatalyst at 600℃ manifested the highest activity. Characterization with UV-visible spectra, XRD, SEM, and XPS revealed that the effect of the Au nanoparticle size and Au-TiO₂ interaction were both responsible for the increase in plasmon-induced water oxidation activity.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

金纳米粒子的尺寸以及金-二氧化钛相互作用对表面等离激元光催化产氧的影响

English

Effects of Au nanoparticle size and metal-support interaction on plasmon-induced photocatalytic water oxidation

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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中国化学会秘书处

金纳米粒子的尺寸以及金-二氧化钛相互作用对表面等离激元光催化产氧的影响

English

Effects of Au nanoparticle size and metal-support interaction on plasmon-induced photocatalytic water oxidation

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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