Pt Single Atoms and Nanosized Clusters as Catalytic Reaction Platforms for Selective Hydrogenation Applications

被引：7

作者：

Xu, Enze ^{[1
]}

Feng, Haisong ^{[1
]}

Wang, Lei ^{[1
]}

Zhang, Yuanjing ^{[1
]}

Liu, Kelong ^{[1
]}

Cui, Shuai ^{[1
]}

Meng, Hao ^{[1
]}

Wang, Guirong ^{[1
]}

Yang, Yusen ^{[1
]}

机构：

[1] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

来源：

ACS APPLIED NANO MATERIALS | 2023年 / 6卷 / 16期

基金：

中国国家自然科学基金; 北京市自然科学基金;

关键词：

single atom; nanosized cluster; selective hydrogenation; unsaturated aldehydes; structure-selectivitycorrelation; TOTAL-ENERGY CALCULATIONS; OXIDATION; ALLOY; FACET; NI;

D O I：

10.1021/acsanm.3c02543

中图分类号：

TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

The exploitation and design of high-efficiency catalystshave attractedextensive attention in the selective regulation of hydrogenation reactions;however, it remains a tremendous challenge currently. Herein, we reporttwo kinds of nanosized Pt-based catalysts, including single-atom catalysts(SACs) and nanosized cluster catalysts (NCCs), anchored onto a CoAlO x support via the topotactic transformationof layered double hydroxides. The SAC (Pt-1/CoAlO x ) exhibits a >99% selectivity toward the hydrogenationof furfural (FAL) to furfuryl alcohol (FOL), while the NCC (Pt- n /CoAlO x ) showsa >99% selectivity for tetrahydrofurfuryl alcohol (THFOL) underamild reaction condition (room temperature and a 0.1 MPa pressure ofH(2)). Both in situ experiments and theoretical calculationsreveal that the aggregation state (single atom or nanosized cluster)of Pt atoms influences the adsorption configuration of FAL, in whichthe adsorption of C O occurs on Pt single atoms over Pt-1/CoAlO x and the adsorption ofboth C C and C O occurs on continuous Pt atoms overPt( n )/CoAlO x . The structure-selectivity relationship substantiates thatmetal ensemble size has an important effect on the adsorption structureof the reaction substrate and thus results in the different selectivityof the hydrogenation reaction.

引用

页码：14991 / 15001

页数：11

共 49 条

[11] Pt/Fe2O3 with Pt-Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading [J].

Gao, Ruijie ;

Wang, Jian ;

Huang, Zhen-Feng ;

Zhang, Rongrong ;

Wang, Wei ;

Pan, Lun ;

Zhang, Junfeng ;

Zhu, Weikang ;

Zhang, Xiangwen ;

Shi, Chengxiang ;

Lim, Jongwoo ;

Zou, Ji-Jun .

NATURE ENERGY, 2021, 6 (06) :614-623

[12] Bimetallic PtFe-Catalyzed Selective Hydrogenation of Furfural to Furfuryl Alcohol: Solvent Effect of Isopropanol and Hydrogen Activation [J].

Gao, Xing ;

Tian, Suyang ;

Jin, Yunyun ;

Wan, Xiaoyue ;

Zhou, Chunmei ;

Chen, Rizhi ;

Dai, Yihu ;

Yang, Yanhui .

ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2020, 8 (33) :12722-12730

[13] A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu [J].

Grimme, Stefan ;

Antony, Jens ;

Ehrlich, Stephan ;

Krieg, Helge .

JOURNAL OF CHEMICAL PHYSICS, 2010, 132 (15)

[14] Low-Temperature Acetylene Semi-Hydrogenation over the Pd1-Cu1 Dual-Atom Catalyst [J].

Huang, Fei ;

Peng, Mi ;

Chen, Yunlei ;

Cai, Xiangbin ;

Qin, Xuetao ;

Wang, Ning ;

Xiao, Dequan ;

Jin, Li ;

Wang, Guoqing ;

Wen, Xiao-Dong ;

Liu, Hongyang ;

Ma, Ding .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (40) :18485-18493

[15] Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set [J].

Kresse, G ;

Furthmuller, J .

PHYSICAL REVIEW B, 1996, 54 (16) :11169-11186

[16] From ultrasoft pseudopotentials to the projector augmented-wave method [J].

Kresse, G ;

Joubert, D .

PHYSICAL REVIEW B, 1999, 59 (03) :1758-1775

[17] Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set [J].

Kresse, G ;

Furthmuller, J .

COMPUTATIONAL MATERIALS SCIENCE, 1996, 6 (01) :15-50

[18] Highly Selective Catalysts for the Hydrogenation of Unsaturated Aldehydes: A Review [J].

Lan, Xiaocheng ;

Wang, Tiefeng .

ACS CATALYSIS, 2020, 10 (04) :2764-2790

[19] Selective hydrogenation of 5-(hydroxymethyl)furfural to 5-methylfurfural over single atomic metals anchored on Nb2O5 [J].

Li, Shaopeng ;

Dong, Minghua ;

Yang, Junjuan ;

Cheng, Xiaomeng ;

Shen, Xiaojun ;

Liu, Shulin ;

Wang, Zhi-Qiang ;

Gong, Xue-Qing ;

Liu, Huizhen ;

Han, Buxing .

NATURE COMMUNICATIONS, 2021, 12 (01)

[20] Decoupling the Interfacial Catalysis of CeO2-Supported Rh Catalysts Tuned by CeO2 Morphology and Rh Particle Size in CO2 Hydrogenation [J].

Liao, Weiqi ;

Yue, Minnan ;

Chen, Junyi ;

Wang, Ziwei ;

Ding, Jieqiong ;

Xu, Yuxing ;

Bai, Yu ;

Liu, Xiaochun ;

Jia, Aiping ;

Huang, Weixin ;

Zhang, Zhenhua .

ACS CATALYSIS, 2023, :5767-5779

← 1 2 3 4 5 →