[2] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[4] State Key Lab Catalysis, Dalian 116023, Peoples R China
来源:
CELL REPORTS PHYSICAL SCIENCE
|
2022年
/
3卷
/
07期
基金:
国家重点研发计划;
中国国家自然科学基金;
关键词:
AMMONIA-SYNTHESIS;
CO OXIDATION;
REDUCTION;
MECHANISM;
HYDRIDES;
D O I:
10.1016/j.xcrp.2022.100970
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
Ammonia is a central vector in sustainable global growth, but the usage of fossil feedstocks and centralized Haber-Bosch synthesis conditions causes >1.4% of global anthropogenic CO2 emissions. While nitrogenase enzymes convert atmospheric N-2 to ammonia at ambient conditions, even the most active manmade inorganic catalysts fail due to low activity and parasitic hydrogen evolution at low temperatures. Here, we show that the [RuH6] catalytic center in ternary ruthenium complex hydrides (Li4RuH6) activates N-2 preferentially and avoids hydrogen over-saturation at low temperatures and near ambient pressure by delicately balancing H-2 chemisorption and N-2 activation. The active [RuH6] catalytic center is capable of achieving high yield at low temperatures via a shift in the rate-determining reaction intermediates and transition states, where the reaction orders in hydrogen and ammonia change dramatically. Temperature-dependent atomic-scale understanding of this unique mechanism is obtained with synchronized experimental and density functional theory investigations.
机构:
College of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, ChinaCollege of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, China
Ji, Sheng-Xiao
Zhang, Wei-Jian
论文数: 0引用数: 0
h-index: 0
机构:
College of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, ChinaCollege of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, China
Zhang, Wei-Jian
Zheng, Yu-Ying
论文数: 0引用数: 0
h-index: 0
机构:
College of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, China
Fujian Chenqi New Material Technology Co., Ltd., Quanzhou,362200, China
Fujian Key Laboratory of Rubber and Plastics New Materials, Quanzhou,362211, ChinaCollege of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, China
Zheng, Yu-Ying
Zhu, Jian-Feng
论文数: 0引用数: 0
h-index: 0
机构:
College of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, ChinaCollege of Materials Science and Engineering, Fuzhou University, Fuzhou,350116, China
Zhu, Jian-Feng
Ranliao Huaxue Xuebao/Journal of Fuel Chemistry and Technology,
2019,
47
(02):
: 224
-
232
机构:
Shanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Wu, Tong
Ren, Shan
论文数: 0引用数: 0
h-index: 0
机构:
Chongqing Univ, Coll Mat Sci & Engn, Chongqing 400044, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Ren, Shan
Guo, Rui-tang
论文数: 0引用数: 0
h-index: 0
机构:
Shanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Shanghai Noncarbon Energy Convers & Utilizat Inst, Shanghai 200090, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Guo, Rui-tang
Li, Chu-fan
论文数: 0引用数: 0
h-index: 0
机构:
Shanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Li, Chu-fan
You, Yi-hao
论文数: 0引用数: 0
h-index: 0
机构:
Shanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
You, Yi-hao
Guo, Shi-yi
论文数: 0引用数: 0
h-index: 0
机构:
Shanghai Elect Power Generat Environm Protect Engn, Shanghai 201612, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Guo, Shi-yi
Pan, Wei-guo
论文数: 0引用数: 0
h-index: 0
机构:
Shanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
Shanghai Noncarbon Energy Convers & Utilizat Inst, Shanghai 200090, Peoples R ChinaShanghai Univ Elect Power, Coll Energy Source & Mech Engn, Shanghai, Peoples R China
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Xu, Qan
Fang, Zhilin
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Fang, Zhilin
Chen, Yiyuan
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Chen, Yiyuan
Guo, Yanglong
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Guo, Yanglong
Guo, Yun
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Guo, Yun
Wang, Li
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Wang, Li
Wang, Yunsong
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Wang, Yunsong
Zhang, Jinshui
论文数: 0引用数: 0
h-index: 0
机构:
Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
Zhang, Jinshui
Zhan, Wangcheng
论文数: 0引用数: 0
h-index: 0
机构:
East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R ChinaEast China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Hu, Wenshuo
Zou, Renzhi
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Zou, Renzhi
Dong, Yi
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Dong, Yi
Zhang, Shuo
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Zhang, Shuo
Song, Hao
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Song, Hao
Liu, Shaojun
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Liu, Shaojun
Zheng, Chenghang
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Zheng, Chenghang
Nova, Isabella
论文数: 0引用数: 0
h-index: 0
机构:
Politecn Milan, Dipartimento Energia, Lab Catalysis & Catalyt Proc, Via La Masa 34, I-20156 Milan, ItalyZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Nova, Isabella
Tronconi, Enrico
论文数: 0引用数: 0
h-index: 0
机构:
Politecn Milan, Dipartimento Energia, Lab Catalysis & Catalyt Proc, Via La Masa 34, I-20156 Milan, ItalyZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China
Tronconi, Enrico
Gao, Xiang
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R ChinaZhejiang Univ, State Key Lab Clean Energy Utilizat, 38 Zheda Rd, Hangzhou 310027, Peoples R China