Visible-light-driven selective alcohol dehydrogenation and hydrogenolysis via the Mott Schottky effect

doi:10.1039/c9ta13811k

	Visible-light-driven selective alcohol dehydrogenation and hydrogenolysis via the Mott Schottky effect
	Yang, Xue 1,2; Zhang, Suyuan1,2,5 ; Tao, Huilin 3,4; Yan, Xuyan 1,3; Tan, Yanxi 1,2; Zhang, Yongfan 3; Gao, Shuiying 1,2; Cao, Rong 1,2,3
	2020-04-14
发表期刊	JOURNAL OF MATERIALS CHEMISTRY A (IF:10.7[JCR-2023],10.8[5-Year])
ISSN	2050-7488
EISSN	2050-7496
卷号	8 期号:14 页码:6854-6862
发表状态	已发表
DOI	10.1039/c9ta13811k
摘要	The Schottky barrier created at the interface between electron sinks and semiconductors can effectively optimize electron transfer for active photocatalysis. However, heterogeneous photocatalytic organic transformations via the Mott Schottky effect are still rare and their role in the specific photocatalytic system remains ambiguous. Here, a versatile photocatalytic system integrating the Schottky junctions into the TiO2 particles (Degussa, P25) and Pd NP based films has been developed. They were readily available through the facile encapsulation of P25 by Pd-H4BINDI films using an alternating layer-by-layer (LBL) approach (H4BINDI: N,N '-bis(5-isophthalate acid)naphthalene-diimide). After a H-2 reduction process under 200 degrees C, the Pd NPs were obtained, denoted as P25@Pd-H4BINDI-200. Interestingly, the resulting P25@Pd-H4BINDI-200 photocatalyst presented an exceptionally high activity for dehydrogenation and hydrogenolysis of benzyl alcohol under visible light irradiation, which was approximately 17 times higher than that of the parent P25@Pd-H4BINDI and was superior to any other analogous systems reported to date. Specifically, the negative charges accumulated on the Pd NP surface reduce the benzyl alcohol, while the holes left on the valence band oxidize the benzyl alcohol, effectively promoting photocatalytic cycles with enhanced carrier separation. The deeper understanding of the reaction mechanisms revealed that Pd NPs play a vital mediating role in storing and shuttling photogenerated electrons via the Mott Schottky effect, and revealed the highly enhanced carrier separation by direct use of photoexcited electrons and holes for photoredox reactions. This work holds great promise for designing Mott-Schottky catalysts in enabling solar-driven photoredox reactions.
收录类别	SCI ; SCIE ; EI
语种	英语
资助项目	Strategic Priority Research Program of the Chinese Academy of Sciences[XDB20000000]
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号	WOS:000526953200040
出版者	ROYAL SOC CHEMISTRY
EI入藏号	20201608418538
EI主题词	Dehydrogenation ; Electrons ; Hydrogenolysis ; Hydrolysis ; Light ; Naphthalene ; Schottky barrier diodes ; Titanium dioxide
EI分类号	Precious Metals:547.1 ; Semiconductor Devices and Integrated Circuits:714.2 ; Light/Optics:741.1 ; Chemical Reactions:802.2 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2
WOS关键词	METAL NANOPARTICLES ; AROMATIC ALCOHOLS ; COUPLING REACTION ; PD ; TIO2 ; EFFICIENT ; PHOTOCATALYSIS ; OXIDATION ; GENERATION ; REDUCTION
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/119543
专题	物质科学与技术学院_博士生
通讯作者	Gao, Shuiying; Cao, Rong
作者单位	1.Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Fuzhou Univ, Coll Chem, Fuzhou 350108, Peoples R China 4.Shangrao Normal Univ, Sch Chem & Environm Sci, Shangrao 334000, Peoples R China 5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
推荐引用方式 GB/T 7714	Yang, Xue,Zhang, Suyuan,Tao, Huilin,et al. Visible-light-driven selective alcohol dehydrogenation and hydrogenolysis via the Mott Schottky effect[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(14):6854-6862.
APA	Yang, Xue.,Zhang, Suyuan.,Tao, Huilin.,Yan, Xuyan.,Tan, Yanxi.,...&Cao, Rong.(2020).Visible-light-driven selective alcohol dehydrogenation and hydrogenolysis via the Mott Schottky effect.JOURNAL OF MATERIALS CHEMISTRY A,8(14),6854-6862.
MLA	Yang, Xue,et al."Visible-light-driven selective alcohol dehydrogenation and hydrogenolysis via the Mott Schottky effect".JOURNAL OF MATERIALS CHEMISTRY A 8.14(2020):6854-6862.