Removal of Hydrogen Poisoning by Electrostatically Polar MgO Support for Low-Pressure NH3 Synthesis at a High Rate over the Ru Catalyst

被引：91

作者：

Wu, Simson ^{[1
]}

Peng, Yung-Kang ^{[1
]}

Chen, Tian-Yi ^{[1
]}

Mo, Jiaying ^{[1
]}

Large, Alex ^{[2
]}

Mcpherson, Ian ^{[1
]}

Chou, Hung-Lung ^{[3
]}

Wilkinson, Ian ^{[4
]}

Venturini, Federica ^{[5
]}

Grinter, David ^{[5
]}

Escorihuela, Pilar Ferrer ^{[5
]}

Held, Georg ^{[2
,5
]}

Tsang, Shik Chi Edman ^{[1
]}

机构：

[1] Univ Oxford, Wolfson Catalysis Ctr, Dept Chem, Oxford OX1 3QR, England

[2] Univ Reading, Reading RG6 6UR, Berks, England

[3] Natl Taiwan Univ Sci & Technol, Grad Inst Appl Sci & Technol, Taipei 10617, Taiwan

[4] Siemens Plc, CT NTF, Oxford OX29 4BP, England

[5] Diamond Light Source, Didcot OX11 0DE, Oxon, England

来源：

ACS CATALYSIS | 2020年 / 10卷 / 10期

基金：

英国工程与自然科学研究理事会;

关键词：

ammonia synthesis; hydrogen poisoning; electrostatically polar surface; proton capture; nanocatalysts; AMMONIA-SYNTHESIS; RUTHENIUM CATALYSTS; METAL-OXIDES; PROMOTERS; KINETICS;

D O I：

10.1021/acscatal.0c00954

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：

The increasing availability of low-cost and low pressure, renewable H-2 from wind and solar means has triggered tremendous interest in developing low pressure ammonia synthesis with N-2 as the energy carrier as well as fertilizer. As such, Cs-promoted Ru/MgO catalysts used in the Kellogg process show superiority to Fe-based catalysts at milder conditions; however, as known, the surface poisoning of Ru sites by competitive strong H-2 dissociative adsorption limits the overall rate. In this study, it is demonstrated that the use of simple electrostatically polar MgO(111) to replace nonpolar MgO as the support can significantly alleviate the hydrogen poisoning and facilitate an unprecedented ammonia production rate by its high intrinsic proton capture ability.

引用

页码：5614 / 5622

页数：9

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