Ting Liu, Zhuo Xiong, Shengnan Deng, Han Wu, Xianhong Wang, Yuhan Huang, Zizhen Ma, Yan Tan, Huawei Zhang
{"title":"碳气凝胶深度去除天然气中的 COS 和 Hg0:0.9PPD-Cu/CA 吸附剂在低温条件下的良好防毒性能和协同效应。","authors":"Ting Liu, Zhuo Xiong, Shengnan Deng, Han Wu, Xianhong Wang, Yuhan Huang, Zizhen Ma, Yan Tan, Huawei Zhang","doi":"10.1021/acs.est.4c09301","DOIUrl":null,"url":null,"abstract":"<p><p>A collaborative COS conversion of Hg<sup>0</sup> in natural gas on the nitrogen-doped and copper oxide-supported carbon aerogel (0.9PPD-Cu/CA), which is synthesized by the <i>p</i>-phenylenediamine sources and carbon source of sodium alginate, was proposed to overcome the easy deactivation of the catalyst, high reaction temperature, and limited lifespan. At 40 °C, the 0.9PPD-Cu/CA presented a 100% COS conversion efficiency in the presence of H<sub>2</sub>O; meanwhile, the N doping realized the enhancement of basic density, leading to an improved COS conversion, and the intermediates H<sub>2</sub>S in the reaction were wholly adsorbed, implying that 0.9PPD-Cu/CA was a bifunctional carbon material. Furthermore, the Hg<sup>0</sup> addition achieved a synergistic performance as well as higher COS yield and a significant lifetime period, in which the sulfur immediate could have a high reactive activity for Hg<sup>0</sup> and the sulfate proportion would be alleviated as well. Subsequently, the catalyst poisoning would be alleviated after the protection of the collaborative process by strengthening the electron transfer, consuming the sulfur-based products, and accelerating the cleavage of the H-S bond. Finally, the synergetic mechanism on COS and Hg<sup>0</sup> on 0.9PPD-Cu/CA was concluded according to the experimental results and sample analysis. Additionally, the effects of space velocity and the regeneration performance were explored.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20598-20606"},"PeriodicalIF":10.8000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Deep Removal of COS and Hg<sup>0</sup> by Carbon Aerogel in Natural Gas: Good Antipoisoning Properties as well as Synergy Effect at Low Temperatures on 0.9PPD-Cu/CA Adsorbent.\",\"authors\":\"Ting Liu, Zhuo Xiong, Shengnan Deng, Han Wu, Xianhong Wang, Yuhan Huang, Zizhen Ma, Yan Tan, Huawei Zhang\",\"doi\":\"10.1021/acs.est.4c09301\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>A collaborative COS conversion of Hg<sup>0</sup> in natural gas on the nitrogen-doped and copper oxide-supported carbon aerogel (0.9PPD-Cu/CA), which is synthesized by the <i>p</i>-phenylenediamine sources and carbon source of sodium alginate, was proposed to overcome the easy deactivation of the catalyst, high reaction temperature, and limited lifespan. At 40 °C, the 0.9PPD-Cu/CA presented a 100% COS conversion efficiency in the presence of H<sub>2</sub>O; meanwhile, the N doping realized the enhancement of basic density, leading to an improved COS conversion, and the intermediates H<sub>2</sub>S in the reaction were wholly adsorbed, implying that 0.9PPD-Cu/CA was a bifunctional carbon material. Furthermore, the Hg<sup>0</sup> addition achieved a synergistic performance as well as higher COS yield and a significant lifetime period, in which the sulfur immediate could have a high reactive activity for Hg<sup>0</sup> and the sulfate proportion would be alleviated as well. Subsequently, the catalyst poisoning would be alleviated after the protection of the collaborative process by strengthening the electron transfer, consuming the sulfur-based products, and accelerating the cleavage of the H-S bond. Finally, the synergetic mechanism on COS and Hg<sup>0</sup> on 0.9PPD-Cu/CA was concluded according to the experimental results and sample analysis. Additionally, the effects of space velocity and the regeneration performance were explored.</p>\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":\" \",\"pages\":\"20598-20606\"},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"环境科学与技术\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.est.4c09301\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/11/6 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.est.4c09301","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/6 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0
摘要
为了克服催化剂易失活、反应温度高、寿命有限等问题,提出了在对苯二胺为源、海藻酸钠为碳源合成的氮掺杂氧化铜支撑碳气凝胶(0.9PPD-Cu/CA)上协同转化天然气中的Hg0的方法。在 40 ℃ 时,0.9PPD-Cu/CA 在 H2O 存在下的 COS 转化率为 100%;同时,N 掺杂实现了碱密度的增强,从而提高了 COS 转化率,并且完全吸附了反应中间产物 H2S,这意味着 0.9PPD-Cu/CA 是一种双功能碳材料。此外,Hg0 的添加实现了协同增效,提高了 COS 收率并延长了使用寿命,其中硫立即对 Hg0 具有较高的反应活性,硫酸盐的比例也得到缓解。随后,通过加强电子传递、消耗硫基产物和加速 H-S 键的裂解,保护协同过程后催化剂中毒现象将得到缓解。最后,根据实验结果和样品分析,得出了 0.9PPD-Cu/CA 上 COS 和 Hg0 的协同机理。此外,还探讨了空间速度和再生性能的影响。
Deep Removal of COS and Hg0 by Carbon Aerogel in Natural Gas: Good Antipoisoning Properties as well as Synergy Effect at Low Temperatures on 0.9PPD-Cu/CA Adsorbent.
A collaborative COS conversion of Hg0 in natural gas on the nitrogen-doped and copper oxide-supported carbon aerogel (0.9PPD-Cu/CA), which is synthesized by the p-phenylenediamine sources and carbon source of sodium alginate, was proposed to overcome the easy deactivation of the catalyst, high reaction temperature, and limited lifespan. At 40 °C, the 0.9PPD-Cu/CA presented a 100% COS conversion efficiency in the presence of H2O; meanwhile, the N doping realized the enhancement of basic density, leading to an improved COS conversion, and the intermediates H2S in the reaction were wholly adsorbed, implying that 0.9PPD-Cu/CA was a bifunctional carbon material. Furthermore, the Hg0 addition achieved a synergistic performance as well as higher COS yield and a significant lifetime period, in which the sulfur immediate could have a high reactive activity for Hg0 and the sulfate proportion would be alleviated as well. Subsequently, the catalyst poisoning would be alleviated after the protection of the collaborative process by strengthening the electron transfer, consuming the sulfur-based products, and accelerating the cleavage of the H-S bond. Finally, the synergetic mechanism on COS and Hg0 on 0.9PPD-Cu/CA was concluded according to the experimental results and sample analysis. Additionally, the effects of space velocity and the regeneration performance were explored.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.