Ceria-supported ruthenium clusters transforming from isolated single atoms for hydrogen production via decomposition of ammonia

被引：159

作者：

Hu, Xiu-Cui ^{[1
]}

Fu, Xin-Pu ^{[1
]}

Wang, Wei-Wei ^{[1
]}

Wang, Xu ^{[2
]}

Wu, Ke ^{[4
]}

Si, Rui ^{[2
]}

Ma, Chao ^{[3
]}

Jia, Chun-Jiang ^{[1
]}

Yan, Chun-Hua ^{[4
]}

机构：

[1] Shandong Univ, Sch Chem & Chem Engn, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Jinan 250100, Peoples R China

[2] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

[3] Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China

[4] Peking Univ, Beijing Natl Lab Mol Sci, State Key Lab Rare Earth Mat Chem & Applicat, PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Che, Beijing 100871, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2020年 / 268卷 / 268期

基金：

美国国家科学基金会;

关键词：

Ru clusters; Ceria; Ammonia decomposition; Hydrogen; Structure-activity relation; INITIO MOLECULAR-DYNAMICS; COX-FREE HYDROGEN; SELECTIVE SYNTHESIS; GOLD NANOPARTICLES; NH3; DECOMPOSITION; STABLE CATALYSTS; CARBON NANOTUBES; RU NANOPARTICLES; OXIDE CLUSTER; METAL;

D O I：

10.1016/j.apcatb.2019.118424

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Supported cluster catalyst exhibits significant superiority in catalytic performance, but the structure uniformity and reactivity stability of the clusters under harsh conditions remains challenges. Here, we report the synthesis of stable ruthenium (Ru) clusters (ca. 1.5 nm) by reducing Ru single atoms under ammonia atmosphere at 550 degrees C, where the Ru clusters are uniformly dispersed on the surface of ceria. The supported Ru cluster catalysts show outstanding activity for decomposition of ammonia with an extremely high hydrogen yield of 9,924 mmolH(2) g(Ru)(-1) min(-1) at 450 degrees C. Such a value exhibits at least one-order enhancement on the hydrogen formation yield compared to the previously reported results. Through comprehensive in-situ characterizations and temperature programmed desorption by NH3 techniques, we clearly explored the structure-function relation of the Ru/CeO2 catalyst that ceria support itself effectively adsorbed ammonia, meanwhile the Ru clusters stabilized by ceria decomposed ammonia to produce hydrogen.

引用

页数：13

共 59 条

[51] Crystal Plane Effect of Ceria on Supported Copper Oxide Cluster Catalyst for CO Oxidation: Importance of Metal-Support Interaction [J].

Wang, Wei-Wei ;

Yu, Wen-Zhu ;

Du, Pei-Pei ;

Xu, Hui ;

Jin, Zhao ;

Si, Rui ;

Ma, Chao ;

Shi, Shuo ;

Jia, Chun-Jiang ;

Yan, Chun-Hua .

ACS CATALYSIS, 2017, 7 (02) :1313-1329

[52] Thermally Stable and Regenerable Platinum-Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria [J].

Xiong, Haifeng ;

Lin, Sen ;

Goetze, Joris ;

Pletcher, Paul ;

Guo, Hua ;

Kovarik, Libor ;

Artyushkova, Kateryna ;

Weckhuysen, Bert M. ;

Datye, Abhaya K. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (31) :8986-8991

[53] Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis [J].

Yang, Xiao-Feng ;

Wang, Aiqin ;

Qiao, Botao ;

Li, Jun ;

Liu, Jingyue ;

Zhang, Tao .

ACCOUNTS OF CHEMICAL RESEARCH, 2013, 46 (08) :1740-1748

[54] Investigation on the catalysis of COx-free hydrogen generation from ammonia [J].

Yin, SF ;

Zhang, QH ;

Xu, BQ ;

Zhu, WX ;

Ng, CF ;

Au, CT .

JOURNAL OF CATALYSIS, 2004, 224 (02) :384-396

[55] The XAFS beamline of SSRF [J].

于海生 ;

魏向军 ;

李炯 ;

顾颂琦 ;

张硕 ;

汪丽华 ;

马静远 ;

李丽娜 ;

高倩 ;

司锐 ;

孙凡飞 ;

王宇 ;

宋飞 ;

徐洪杰 ;

余笑寒 ;

邹杨 ;

王建强 ;

姜政 ;

黄宇营 .

NuclearScienceandTechniques, 2015, 26 (05) :6-12

[56] Facile synthesis for ordered mesoporous γ-aluminas with high thermal stability [J].

Yuan, Quan ;

Yin, An-Xiang ;

Luo, Chen ;

Sun, Ling-Dong ;

Zhang, Ya-Wen ;

Duan, Wen-Tao ;

Liu, Hai-Chao ;

Yan, Chun-Hua .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (11) :3465-3472

[57] Catalytic activities of CeO2(110)-2 x 1 reconstructed surface [J].

Zhang, Jie ;

Gong, Xue-Qing ;

Lu, Guanzhong .

SURFACE SCIENCE, 2015, 632 :164-173

[58] Mechanism of selective catalytic oxidation of ammonia to nitrogen over Ag/Al2O3 [J].

Zhang, Li ;

He, Hong .

JOURNAL OF CATALYSIS, 2009, 268 (01) :18-25

[59] Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition [J].

Zheng, Weiqing ;

Cotter, Thomas P. ;

Kaghazchi, Payam ;

Jacob, Timo ;

Frank, Benjamin ;

Schlichte, Klaus ;

Zhang, Wei ;

Su, Dang Sheng ;

Schueth, Ferdi ;

Schloegl, Robert .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (09) :3458-3464

← 1 2 3 4 5 6 →