Site-specific photocatalytic splitting of methanol on TiO2(110)

Chuanyao Zhou; Zefeng Ren; Shijing Tan; Zhibo Ma; Xinchun Mao; Dongxu Dai; Hongjun Fan; Xueming Yang; Jerry LaRue; Russell Cooper; Alec M. Wodtke; Zhuo Wang; Zhenyu Li; Bing Wang; Jinlong Yang; Jianguo Hou

doi:10.1039/C0SC00316F

Site-specific photocatalytic splitting of methanol on TiO₂(110)†

Chuanyao Zhou,‡^a Zefeng Ren,‡^a Shijing Tan,‡^a Zhibo Ma,^a Xinchun Mao,^a Dongxu Dai,^a Hongjun Fan,*^a Xueming Yang,*^a Jerry LaRue,^b Russell Cooper,^b Alec M. Wodtke,^b Zhuo Wang,^c Zhenyu Li,^c Bing Wang,*^c Jinlong Yang^c and Jianguo Hou^c

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* Corresponding authors

^a State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, 457 Zhongshan Road, Dalian, Liaoning, P. R. China
E-mail: fanhj@dicp.ac.cn, xmyang@dicp.ac.cn

^b Department of Chemistry and Biochemistry, University of California at Santa Barbara, CA, USA

^c Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, China
E-mail: bwang@ustc.edu

Abstract

Clean hydrogen production is highly desirable for future energy needs, making the understanding of molecular-level phenomena underlying photocatalytic hydrogen production both fundamentally and practically important. Water splitting on pure TiO₂ is inefficient, however, adding sacrificial methanol could significantly enhance the photocatalyzed H₂ production. Therefore, understanding the photochemistry of methanol on TiO₂ at the molecular level could provide important insights to its photocatalytic activity. Here, we report the first clear evidence of photocatalyzed splitting of methanol on TiO₂ derived from time-dependent two-photon photoemission (TD-2PPE) results in combination with scanning tunneling microscopy (STM). STM tip induced molecular manipulation before and after UV light irradiation clearly reveals photocatalytic bond cleavage, which occurs only at Ti⁴⁺ surface sites. TD-2PPE reveals that the kinetics of methanol photodissociation is clearly not of single exponential, an important characteristic of this intrinsically heterogeneous photoreaction.

Chemical Science

Site-specific photocatalytic splitting of methanol on TiO₂(110)†

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Site-specific photocatalytic splitting of methanol on TiO₂(110)

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