Potential Risk of NH3 Slip Arisen from Catalytic Inactive Site in Selective Catalytic Reduction of NOx with Metal-Free Carbon

被引:18
作者
Yuan, Jin [1 ]
Wang, Zhen [1 ]
Liu, Jun [2 ]
Li, Junhua [1 ]
Chen, Jianjun [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100084, Peoples R China
[2] Taiyuan Univ Technol, Coll Chem, Taiyuan 030024, Peoples R China
基金
中国国家自然科学基金;
关键词
NH3; slip; NH3-SCR; carbon catalysts; inactive sites; regeneration; OXIDATION; NANOTUBES; DEHYDROGENATION; TEMPERATURE; NITROGEN; AMMONIA;
D O I
10.1021/acs.est.2c06289
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Ammonia emissions from industrial processes have rapidly increased in the past years. Recent advances have used carbon-based selective catalytic reduction (SCR) technology combined with a reaction-regeneration process to reduce NOx from sintering flue gas, while NH3 slip is seldom accounted for in this process. This study demonstrates that although the electrophilic carboxyl groups (-COOH) on metal-free carbon catalysts exhibit strong adsorption toward NH3, they do not participate in the SCR reaction. As a result of the competitive adsorption of NH3 in the reaction step, these catalytic inactive carboxyl groups not only prolong the time to the SCR steady state, but also result in the potential risk of NH3 slip. A linear relationship with the equimolar ratio between carboxyl groups and slipped NH3 was established in the regeneration steps. The slip of NH3 could be alleviated by the decomposition of carboxyl groups, and special attention should be paid to the presence of inactive sites with strong NH3 adsorption on industrial-employed carbon catalysts. In addition to advancing the understanding of the NH3-SCR mechanism, this work also provides valuable opportunities for the control of ammonia emissions from industrial processes.
引用
收藏
页码:606 / 614
页数:9
相关论文
共 36 条
[1]   Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation [J].
Abednatanzi, Sara ;
Derakhshandeh, Parviz Gohari ;
Leus, Karen ;
Vrielinck, Henk ;
Callens, Freddy ;
Schmidt, Johannes ;
Savateev, Aleksandr ;
Van der Voort, Pascal .
SCIENCE ADVANCES, 2020, 6 (14)
[2]   Vanadium loaded carbon-based monoliths for the on-board no reduction: Influence of temperature and period of the oxidation treatment [J].
Boyano, A. ;
Herrera, C. ;
Larrubia, M. A. ;
Alemany, L. J. ;
Moliner, R. ;
Lazaro, M. J. .
CHEMICAL ENGINEERING JOURNAL, 2010, 160 (02) :623-633
[3]   Catalytic wet air oxidation of phenol over carbon nanotubes: Synergistic effect of carboxyl groups and edge carbons [J].
Cao, Yonghai ;
Li, Bo ;
Zhong, Guoyu ;
Li, Yuhang ;
Wang, Hongjuan ;
Yu, Hao ;
Peng, Feng .
CARBON, 2018, 133 :464-473
[4]   Assessing Contributions of Agricultural and Nonagricultural Emissions to Atmospheric Ammonia in a Chinese Megacity [J].
Chang, Yunhua ;
Zou, Zhong ;
Zhang, Yanlin ;
Deng, Congrui ;
Hu, Jianlin ;
Shi, Zhihao ;
Dore, Anthony J. ;
Collett, Jeffrey L., Jr. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2019, 53 (04) :1822-1833
[5]   Competitive Uptake of Dimethylamine and Trimethylamine against Ammonia on Acidic Particles in Marine Atmospheres [J].
Chen, Dihui ;
Yao, Xiaohong ;
Chan, Chak Keung ;
Tian, Xiaomeng ;
Chu, Yangxi ;
Clegg, Simon Leslie ;
Shen, Yanjie ;
Gao, Yang ;
Gao, Huiwang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (09) :5430-5439
[6]   Rapid Increase in China's Industrial Ammonia Emissions: Evidence from Unit-Based Mapping [J].
Chen, Yuang ;
Zhang, Qianru ;
Cai, Xingrui ;
Zhang, Haoran ;
Lin, Huiming ;
Zheng, Chaoyue ;
Guo, Zhanqiang ;
Hu, Shanying ;
Chen, Long ;
Tao, Shu ;
Liu, Maodian ;
Wang, Xuejun .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (06) :3375-3385
[7]   Insight into the Transformation Behaviors of Dioxins from SinteringFlue Gas in the Cyclic Thermal Regeneration by the V2O5/ACCatalyst-sorbent [J].
Ding, Xiaoxiao ;
Yang, Yatao ;
Zeng, Zequan ;
Huang, Zhanggen .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (09) :5786-5795
[8]   Assessing the Nature of Active Sites on Nanodiamonds as Metal-Free Catalysts for the EB-to-ST Direct Dehydrogenation Using a Catalytic Approach [J].
Feng, Lu ;
Ali, Sajjad ;
Xu, Chi ;
Cao, Shuo ;
Tuci, Giulia ;
Giambastiani, Giuliano ;
Pham-Huu, Cuong ;
Liu, Yuefeng .
ACS CATALYSIS, 2022, 12 (10) :6119-6131
[9]   Abating ammonia is more cost-effective than nitrogen oxides for mitigating PM2.5 air pollution [J].
Gu, Baojing ;
Zhang, Lin ;
Van Dingenen, Rita ;
Vieno, Massimo ;
Van Grinsven, Hans J. M. ;
Zhang, Xiuming ;
Zhang, Shaohui ;
Chen, Youfan ;
Wang, Sitong ;
Ren, Chenchen ;
Rao, Shilpa ;
Holland, Mike ;
Winiwarter, Wilfried ;
Chen, Deli ;
Xu, Jianming ;
Sutton, Mark A. .
SCIENCE, 2021, 374 (6568) :758-+
[10]   Vehicular Emissions Enhanced Ammonia Concentrations in Winter Mornings: Insights from Diurnal Nitrogen Isotopic Signatures [J].
Gu, Mengna ;
Pan, Yuepeng ;
Walters, Wendell W. ;
Sun, Qian ;
Song, Linlin ;
Wang, Yuesi ;
Xue, Yifeng ;
Fang, Yunting .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (03) :1578-1585