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Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light

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成果类型:
期刊论文
作者:
Mao, Chengliang;Li, Hao;Gu, Honggang;Wang, Jiaxian;Zou, Yunjie;...
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Hao; Shen, Wenjuan; Zou, Yunjie; Wang, Jiaxian; Mao, Chengliang; Zhao, Jincai; Li, Jie] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
[Gu, Honggang; Liu, Shiyuan] Huazhong Univ Sci & Technol, State Key Lab Digital Mfg Equipment & Technol, Wuhan 430074, Hubei, Peoples R China.
[Qi, Guodong; Xu, Jun; Deng, Feng] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, CAS Key Lab Magnet Resonance Biol Syst, Wuhan Inst Phys & Math,Natl Ctr Magnet Resonance, Wuhan 430071, Hubei, Peoples R China.
通讯机构:
[Zhang, Lizhi] C
Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
语种:
英文
关键词:
ammonia synthesis;black TiO2;equilibrium limit;Fe nanonecklace;nitrogen fixation;oxygen vacancy;photocatalysis;photothermal catalysis;plasmonic;SDG7: Affordable and clean energy;TiO2
期刊:
Chem
ISSN:
2451-9294
年:
2019
卷:
5
期:
10
页码:
2702-2717
基金类别:
This work was supported by National Natural Science Funds for Distinguished Young Scholars (21425728), National Key Research and Development Program of China (2016YFA0203002), National Science Foundation of China (51472100, 21872061, 51727809, and 51805193), and Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University (2018YBZZ024). Special thanks to Professor Lan Ling (Tongji University) for performing the high-quality STEM characterizations. We thank Professor Wenfeng Han (Zhejiang University of Technology) for providing the commercial wüstite-based Fe catalyst and helpful discussions about the catalyst loading. We also thank the National Supercomputer Center in Ji'nan and Shenzhen for providing high-performance computation. L.Z. and J.Z. supervised the project. C.M. designed and carried out the study. C.M. J.W. Y.Z. and S.W. conducted the experiments. H.G. and S.L. measured optical constants of the material. C.M. performed DFT calculation and FDTD simulation. G.Q. J.X. and F.D. performed EPR simulation and analysis. C.M. L.Z. H.L. and J.Z. co-wrote the manuscript. All authors discussed the results and commented on the manuscript. The authors declare no competing interests. L.Z. and C.M. have applied for a US patent, which has been granted (no. 10,112,841), and a provisional Chinese patent related to this work.
机构署名:
本校为第一且通讯机构
院系归属:
化学学院
摘要:
Plasmonic local heating effect of Fe nanonecklace endowed TiO2-xHy/Fe catalyst of hot-zone Fe and cool-zone TiO2-xHy, which were responsible for tandem N2 activation and NH3 assembly, respectively. With such dual temperature zones and the tandem kinetic mechanism, light-driven TiO2-xHy/Fe nanonecklace achieved highly efficient ammonia synthesis with NH3 yield beyond the thermodynamic equilibrium limit of thermocatalytic ammonia synthesis. © 2019 Elsevier Inc.Artificial ammonia synthesis (Haber-Bosch process) is a prototypical exothermic reacti...

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