Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants

doi:10.1039/c9nr09534a

	Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants
	Bao, Haoming 1; Zhu, Shuyi 1,2; Zhou, Le 1,2; Fu, Hao 1,2; Zhang, Hongwen 1; Cai, Weiping 1,2
刊名	NANOSCALE
	2020-02-14
卷号	12
ISSN号	2040-3364
DOI	10.1039/c9nr09534a
通讯作者	Zhang, Hongwen(hwzhang@issp.ac.cn) ; Cai, Weiping(wpcai@issp.ac.cn)
英文摘要	Blackening (or enhancing the optical absorption in the visible region) of nano-sized white semiconducting oxides (N-WSOs) is of significant importance for solar utilization. Here, we present a novel Mars-van-Krevelen mechanism-based method for blackening the N-WSOs via facile one-step heating of the N-WSOs with alcohols. Taking n-butanol-induced blackening of TiO2 (anatase) as an example, the pristine TiO2 NP powders can be successfully blackened to form black TiO2 (B-TiO2) via heating with n-butanol at 300 degrees C for 20 min. Technical analyses demonstrate that the B-TiO2 nanocrystals are wrapped with a 2 nm thick disordered layer, which is rich in oxygen vacancies, Ti3+ and hydroxyl groups. Both theoretical and experimental results show that B-TiO2 has much stronger optical absorption in the visible region than pristine TiO2. Furthermore, the influence factors (including heating temperatures and alcohol types) and good universality of this blackening method are also demonstrated. A blackening principle based on Mars-van-Krevelen mechanism-induced oxygen vacancy generation and hydroxylation-anchoring of oxygen vacancies has been proposed, and the mechanism can well explain all the phenomena observed in experiments. Importantly, such B-TiO2 shows hugely enhanced activity in solar photodegradation of dye pollutants. Under simulated solar irradiation, the degradation rate constant achieved by the B-TiO2 catalyst is 2.3 times that of the pristine TiO2, showing an obvious enhancement. Further experiments reveal that the improved degradation activity is mainly attributed to the enhanced optical absorption in the visible region and the synergistic photothermal and photocatalytic effect. This study demonstrates a new and facile approach to blacken the N-WSOs for enhanced solar utilization.
资助项目	National Key Research and Development Program of China[2017YFA0207101] ; National Natural Science Foundation of China[11974352] ; National Natural Science Foundation of China[51771182] ; National Natural Science Foundation of China[51531006] ; Chinese Postdoctoral Science Foundation[2019M662211]
WOS关键词	OPTICAL-PROPERTIES ; ZNO NANOPARTICLES ; TIO2 ; ABSORPTION ; ANATASE ; PHOTOCATALYSIS ; CATALYSTS ; TITANIA ; GROWTH ; RUTILE
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000515391000047
资助机构	National Key Research and Development Program of China ; National Natural Science Foundation of China ; Chinese Postdoctoral Science Foundation
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/103999]
专题	中国科学院合肥物质科学研究院
通讯作者	Zhang, Hongwen; Cai, Weiping
作者单位	1.Chinese Acad Sci, Inst Solid State Phys, Anhui Key Lab Nanomat & Nanotechnol, Key Lab Mat Phys, Hefei 230031, Peoples R China 2.Univ Sci & Technol China, Hefei 230026, Peoples R China
推荐引用方式 GB/T 7714	Bao, Haoming,Zhu, Shuyi,Zhou, Le,et al. Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants[J]. NANOSCALE,2020,12.
APA	Bao, Haoming,Zhu, Shuyi,Zhou, Le,Fu, Hao,Zhang, Hongwen,&Cai, Weiping.(2020).Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants.NANOSCALE,12.
MLA	Bao, Haoming,et al."Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants".NANOSCALE 12(2020).