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CVOCs催化燃烧&CeO2基催化剂取得进展发表于Environmental Science & Technology

已有 528 次阅读 2021-2-24 08:28 |个人分类:科研点滴启发|系统分类:科研笔记

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感谢邓博士,郭利民教授,瞻望成教授的支持;感谢编辑部及审稿人的付出。

Abstract: Bulk metal doping and surface phosphate modification were synergically adopted in a rational design to upgrade CeO2 catalyst, which is highly active but easily deactivated for the catalytic oxidation of chlorinated volatile organic compounds (Cl-VOCs). The metal doping increased the redox ability and defect sites of CeO2, which mostly promoted catalytic activity and inhibited the formation of dechlorinated by-products but generated polychlorinated by-products. The subsequent surface modification of the metal-doped CeO2 catalysts with non-metallic phosphate completely suppressed the formation of polychlorinated by-products, and more importantly, enhanced the stability of the surface structure by forming a chainmail layer. A highly active, durable, and selective catalyst of phosphate-functionalised RuOx–CeO2 was the most promising among all the metal-doped (Ru, Pd, Pt, Cr, Mn, Fe, Co, and Cu)-CeO2 catalysts investigated owing to the prominent chemical stability of RuOx and its superior versatility in the catalytic oxidation of different kinds of Cl-VOCs as well as other typical pollutants, including dimethyl sulfide, CO, and C3H8. Moreover, the chemical stability of the catalyst, including its bulk and surface structural stability, was investigated by combining intensive treatment with HCl/H2O or HCl with subsequent ex-situ ultraviolet–visible light Raman spectroscopy, and confirmed the superior resistance to Cl poisoning of the phosphate-functionalised RuOx–CeO2. This work exemplifies a promising strategy for developing idea catalysts for the removal of Cl-VOCs, and provides a catalyst with the superior catalytic performance in Cl-VOCs oxidation to date.

Keywords: Chlorinated volatile organic compounds; Catalytic combustion; Ceria; Chemical stability; Selectivity

文章先睹为快(另外一个版本的,与正式发表的有点不一样,虽然数据一样但是体现的思想不一样,有兴趣的可以看看)

原始版本.pdf


经过优化的氧化铈基催化剂对于VOCs的催化燃烧“接近完美”,具有高活性、稳定性、选择性、广谱性(但是还有一个小缺点,希望在下一篇文章中解决)

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后续还有一篇系列文章,完成了一半工作量了,也估计是CeO2系列的最后一篇了

[1] Qiguang Dai, Xingyi Wang, Guanzhong Lu, Low-temperature catalytic destruction of chlorinated VOCs over cerium oxide, Catalysis Communications, 8 (2007) 1645-1649.

[2] Qiguang Dai, Xingyi Wang, Guanzhong Lu, Low-temperature catalytic combustion of trichloroethylene over cerium oxide and catalyst deactivation, Applied Catalysis B: Environmental, 81 (2008) 192-202.

[3] Hongfeng Li, Guanzhong Lu, Qiguang Dai, Yanqin Wang, Yun Guo, Yanglong Guo, Hierarchical Organization and Catalytic Activity of High-Surface-Area Mesoporous Ceria Microspheres Prepared Via Hydrothermal Routes, ACS Appl. Mater. Interfaces, 2 (2010) 838-846.

[4] Hongfeng Li, Guanzhong Lu, Qiguang Dai, Yanqin Wang, Yun Guo, Yanglong Guo, Efficient Low-temperature Catalytic Combustion of Trichloroethylene over Flower-like Mesoporous Mn-doped CeO2 Microspheres, Applied Catalysis B: Environmental, 102(2011) 475-483.

[5] Qiguang Dai, Hao Huang, Yu Zhu, Wei Deng, Shuxing Bai, Xingyi Wang, Guanzhong Lu, Catalysis oxidation of 1, 2-dichloroethane and ethyl acetate over ceria nanocrystals with well-defined crystal planes, Applied Catalysis B: Environmental, 117 (2012) 360-368.

[6] Qiguang Dai, Shuxing Bai, Zhengyi Wang, Xingyi Wang, Guanzhong Lu, Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts, Applied Catalysis B: Environmental, 126 (2012) 64-75.

[7] Qiguang Dai, Shuxing Bai, Xingyi Wang, Guanzhong Lu, Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts: Mechanism study, Applied Catalysis B: Environmental, 129 (2013) 580-588.

[8] Qiguang Dai, Shuxing Bai, Jianwei Wang, Meng Li, Xingyi Wang, Guanzhong Lu, The effect of TiO2 doping on catalytic performances of Ru/CeO2 catalysts during catalytic combustion of chlorobenzene, Applied Catalysis B: Environmental, 142 (2013) 222-233.

[9] Qiguang Dai, Shuxing Bai, Hua Li, Wei Liu, Xingyi Wang, Guanzhong Lu, Template-free and non-hydrothermal synthesis of CeO2 nanosheets via a facile aqueous-phase precipitation route with catalytic oxidation properties, CrystEngComm, 16 (2014) 9817-9827.

[10] Qiguang Dai, Shuxing Bai, Hua Li, Wei Liu, Xingyi Wang, Guanzhong Lu, Catalytic total oxidation of 1, 2-dichloroethane over highly dispersed vanadia supported on CeO2 nanobelts, Applied Catalysis B: Environmental, 168 (2015) 141-155.

[11] Qiguang Dai, Li-Li Yin, Shuxing Bai, Wei Wang, Xingyi Wang, Xue-Qing Gong, Guanzhong Lu, Catalytic total oxidation of 1, 2-dichloroethane over VOx/CeO2 catalysts: Further insights via isotopic tracer techniques, Applied Catalysis B: Environmental, 182 (2016) 598-610.

[12] Qiguang Dai, , Wei Wang, Xingyi Wang, , Guanzhong Lu, Sandwich-structured CeO2@ZSM-5 hybrid composites for catalytic oxidation of 1, 2-dichloroethane: An integrated solution to coking and chlorine poisoning deactivation, Applied Catalysis B: Environmental, Volume 203, April 2017, Pages 31–42

[13] Wei Wang, Qin Zhu, Qiguang Dai*,  Xingyi Wang,Fe doped CeO2 nanosheets for catalytic oxidation of 1, 2-dichloroethane: Effect of preparation method,Chemical Engineering Journal, 307, 2017, 1037-1046.

[14] Qiguang Dai, Zhiyong Zhang, Jiaorong Yan, Jinyan Wu, Grayson Johnson, Wei Sun, Xingyi Wang, Sen Zhang, Wangcheng Zhan,Phosphate-Functionalized CeO2 Nanosheets for Efficient Catalytic Oxidation of Dichloromethane Environmental science & technology,2018, 52 (22), 13430-13437

[15] Qiguang Dai, Jinyan Wu, Wei Deng, Jiasu Hu, Qingqing Wu, Limin Guo, Wei Sun, Wangcheng Zhan, Xingyi Wang , Comparative studies of P/CeO2 and Ru/CeO2 catalysts for catalytic combustion of dichloromethane: From effects of H2O to distribution of chlorinated by-products, Applied Catalysis B: Environmental, 2019, 249, 9-18

[16] Long Zhang, Wei Deng*, Yuanpu Cai, Qiguang Dai*, and Limin Guo*Comparative Studies of Phosphate-Modified CeO2 and Al2O3 for Mechanistic Understanding of Dichloromethane Oxidation and Chloromethane Formation, ACS Catal. 2020, 10, 21, 13109–13124








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