Effect of Pd and Au on Hydrogen Abstraction and C-C Cleavage in Photoconversion of Glycerol: Beyond Charge Separation

Lv, Dongdong1,2; Lei, Yechen3,4; Zhang, Dongsheng5; Song, Xin4; Li, Yong-Wang4; Niemantsverdriet, J. W. H.4,6; Hao, Weichang1,2; Deng, Yonghong3; Su, Ren4,5

2020-09-17

10.1021/acs.jpcc.0c07148

Journal of Physical Chemistry C   影响因子和分区

1932-7447

1932-7455

Photocatalytic conversion of polyols to value-added products is of great interest for the utilization of biomass as a chemical feedstock. Current research focuses on boosting the reaction rate and selectivity by employing metal nanoparticles (NPs) as charge separators and cocatalysts. However, the promotional role of metal NPs in such photocatalytic processes still remains unclear because of the lack of mechanistic understanding. Here, we have explored the role of supported Pd and Au NPs on TiO2 in photocatalytic glycerol conversion under water-free, deaerated conditions by in situ spectroscopic methods. While the presence of Au NPs only results in partial conversion of glycerol at a low rate, Pd decoration promotes glycerol oxidation to a much higher conversion. In situ mass and vibrational spectrometry reveals that Pd/TiO2 exhibits faster cleavage of O-H and C-H bonds in both glycerol and the derived intermediates as compared to Au/TiO2, thus leading to a higher glycerol conversion accompanied by the formation of additional molecular hydrogen. X-ray photoelectron spectroscopy suggests that the preferential adsorption of glycerol on the surface of Pd via hydroxyl groups results in an enhanced interfacial charge transfer, thus yielding a better photocatalytic activity.

SCI ; EI

英语

通讯

NSFC[21972100][51672018][51472016] ; Beijing Natural Science Foundation[Z180007] ; Fundamental Research Foundation of Shenzhen[JCYJ20170412153424150] ; International Scientific and Technological Cooperation[GJHZ20180411143536149]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000574908200045

AMER CHEMICAL SOC

20204509463635

Spectroscopic analysis ; X ray photoelectron spectroscopy ; Palladium ; Photocatalytic activity ; Gold ; Charge transfer ; Metal nanoparticles ; Hydrogen ; TiO2 nanoparticles ; Titanium dioxide

Precious Metals:547.1 ; Nanotechnology:761 ; Chemistry:801 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2

Web of Science

1.Beihang Univ, Sch Phys, Beijing 100191, Peoples R China
2.Beihang Univ, BUAA UOW Joint Res Ctr, Beijing 100191, Peoples R China
3.Southern Univ Sci & Technol SUSTech, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Synfuels China Technol Co Ltd, SynCat Beijing, Beijing 101407, Peoples R China
5.Soochow Univ, Key Lab Adv Carbon Mat & Wearable Energy Technol, Soochow Inst Energy & Mat Innovat SIEMIS, Suzhou 215006, Peoples R China
6.Syngaschem BV, SynCat DIFFER, NL-6336 HH Eindhoven, Netherlands

Lv, Dongdong,Lei, Yechen,Zhang, Dongsheng,et al. Effect of Pd and Au on Hydrogen Abstraction and C-C Cleavage in Photoconversion of Glycerol: Beyond Charge Separation[J]. Journal of Physical Chemistry C,2020,124(37):20320-20327.

Lv, Dongdong.,Lei, Yechen.,Zhang, Dongsheng.,Song, Xin.,Li, Yong-Wang.,...&Su, Ren.(2020).Effect of Pd and Au on Hydrogen Abstraction and C-C Cleavage in Photoconversion of Glycerol: Beyond Charge Separation.Journal of Physical Chemistry C,124(37),20320-20327.

Lv, Dongdong,et al."Effect of Pd and Au on Hydrogen Abstraction and C-C Cleavage in Photoconversion of Glycerol: Beyond Charge Separation".Journal of Physical Chemistry C 124.37(2020):20320-20327.