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

doi:10.1016/j.chempr.2019.07.021

	Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light
	Mao, Chengliang 3; Li, Hao 3; Gu, Honggang 2; Wang, Jiaxian 3; Zou, Yunjie 3; Qi, Guodong 1; Xu, Jun 1; Deng, Feng 1; Shen, Wenjuan 3; Li, Jie 3
刊名	CHEM
	2019-10-10
卷号	5 期号:10 页码:2702-2717
ISSN号	2451-9294
DOI	10.1016/j.chempr.2019.07.021
英文摘要	Artificial ammonia synthesis (Haber-Bosch process) is a prototypical exothermic reaction of maximum catalytic yield restricted by the unbreakable equilibrium law. This is because bottlenecked N-2 dissociation necessitates high temperature, but high temperature reversely shifts the thermal equilibrium toward NH3 decomposition. To surmount this equilibrium limit, here, we propose a new scenario of dual-temperature-zone catalysis. Powered by sunlight, the apparent temperature of TiO2-xHy/Fe hybrid reaches 495 degrees C but with local temperature difference up to 137 degrees C between the hot zone (Fe) and "cooling" zone (TiO2-xHy) owing to the plasmonic local heating effect. The hot Fe bearing hot carriers efficiently dissociates N-2, while working-in-tandem TiO2-xHy well accommodates spilled-over N from Fe via successive hydrogenation, prominently mitigating the reverse equilibrium shift and thus delivering record NH3 concentrations of 1,939 (1 atm) and 19,620 ppm (10 atm) at 495 degrees C,1.55 and 1.57 times the theoretical equilibrium limits of 1,249 and 12,459 ppm, respectively.
资助项目	National Natural Science Funds for Distinguished Young Scholars[21425728] ; National Key Research and Development Program of China[2016YFA0203002] ; National Science Foundation of China[51472100] ; National Science Foundation of China[21872061] ; National Science Foundation of China[51727809] ; National Science Foundation of China[51805193] ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University[2018YBZZ024]
WOS关键词	MEDIATED NITROGEN TRANSFER ; SURFACE ; DISSOCIATION ; PHOTOCATALYSIS ; CONVERSION ; DIOXIDE ; HYDRIDE ; HYDROGENATION ; PARTICLES ; MECHANISM
WOS研究方向	Chemistry
语种	英语
出版者	CELL PRESS
WOS记录号	WOS:000489631400019
资助机构	National Natural Science Funds for Distinguished Young Scholars ; National Natural Science Funds for Distinguished Young Scholars ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Science Foundation of China ; National Science Foundation of China ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; National Natural Science Funds for Distinguished Young Scholars ; National Natural Science Funds for Distinguished Young Scholars ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Science Foundation of China ; National Science Foundation of China ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; National Natural Science Funds for Distinguished Young Scholars ; National Natural Science Funds for Distinguished Young Scholars ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Science Foundation of China ; National Science Foundation of China ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; National Natural Science Funds for Distinguished Young Scholars ; National Natural Science Funds for Distinguished Young Scholars ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Science Foundation of China ; National Science Foundation of China ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University ; Excellent Doctoral Dissertation Cultivation Grant from Central China Normal University
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/21418]
专题	中国科学院武汉物理与数学研究所
通讯作者	Zhang, Lizhi
作者单位	1.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 2.Huazhong Univ Sci & Technol, State Key Lab Digital Mfg Equipment & Technol, Wuhan 430074, Hubei, Peoples R China 3.Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Mao, Chengliang,Li, Hao,Gu, Honggang,et al. Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light[J]. CHEM,2019,5(10):2702-2717.
APA	Mao, Chengliang.,Li, Hao.,Gu, Honggang.,Wang, Jiaxian.,Zou, Yunjie.,...&Zhang, Lizhi.(2019).Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light.CHEM,5(10),2702-2717.
MLA	Mao, Chengliang,et al."Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light".CHEM 5.10(2019):2702-2717.