{"title":"用于合成多孔富氮碳的可重复使用盐模板策略可促进 H2S 选择性氧化","authors":"Xu Liu, Liang Shan, Xiaoxue Sun, Tianxin Wang, Zhongqing Liu, Yuefeng Liu","doi":"10.1016/j.gee.2024.01.005","DOIUrl":null,"url":null,"abstract":"<p>Removing hydrogen sulfide (H<sub>2</sub>S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H<sub>2</sub>S into elemental sulfur. While N-doped porous carbon was applied to H<sub>2</sub>S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H<sub>2</sub>S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g<sub>sulfur</sub>·kg<sub>cat.</sub><sup>-1</sup>·h<sup>-1</sup>), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO<sub>2</sub> and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"107 1","pages":""},"PeriodicalIF":10.7000,"publicationDate":"2024-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Reusable Salt-template Strategy for Synthesis of Porous Nitrogen-rich Carbon Boosts H2S Selective Oxidation\",\"authors\":\"Xu Liu, Liang Shan, Xiaoxue Sun, Tianxin Wang, Zhongqing Liu, Yuefeng Liu\",\"doi\":\"10.1016/j.gee.2024.01.005\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Removing hydrogen sulfide (H<sub>2</sub>S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H<sub>2</sub>S into elemental sulfur. While N-doped porous carbon was applied to H<sub>2</sub>S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H<sub>2</sub>S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g<sub>sulfur</sub>·kg<sub>cat.</sub><sup>-1</sup>·h<sup>-1</sup>), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO<sub>2</sub> and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.</p>\",\"PeriodicalId\":12744,\"journal\":{\"name\":\"Green Energy & Environment\",\"volume\":\"107 1\",\"pages\":\"\"},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2024-01-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Energy & Environment\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.gee.2024.01.005\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Energy & Environment","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.gee.2024.01.005","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
通过选择性氧化去除硫化氢(H2S)被认为是进一步净化含硫工业的有效方法,因为它可以将残留的 H2S 完全转化为元素硫。虽然掺杂 N 的多孔碳已被应用于 H2S 选择性氧化,但合成高效稳定的掺杂 N 的碳催化剂的可持续方法仍是一个难题,限制了其未来在大规模应用中的发展。在此,我们以可重复使用的 NaCl 为模板,制备了具有大比表面积、高吡啶 N 含量和大量结构缺陷的多孔蜂窝状 N-掺杂碳催化剂,用于 H2S 选择性氧化。所制备的 NC-10-800 催化剂具有优异的催化性能(硫形成率为 784 gsulfur-kgcat.-1-h-1)、出色的稳定性(100 h)以及出色的抗水蒸气、抗 CO2 和抗氧化性能,表明其在实际工业应用中具有巨大潜力。表征结果和动力学研究表明,高温熔盐产生的大表面积和结构缺陷增强了吡啶 N 位点的暴露,从而加快了催化活性。重要的是,水溶性氯化钠模板可以很容易地从碳纳米材料中洗掉,因此下游的含盐废水随后可以重新用于碳前驱体的溶解。这种环境友好型、低成本、可重复使用的盐模板策略对掺杂 N 的碳催化剂的实际应用开发具有重要意义。
Reusable Salt-template Strategy for Synthesis of Porous Nitrogen-rich Carbon Boosts H2S Selective Oxidation
Removing hydrogen sulfide (H2S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H2S into elemental sulfur. While N-doped porous carbon was applied to H2S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H2S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 gsulfur·kgcat.-1·h-1), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO2 and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.
期刊介绍:
Green Energy & Environment (GEE) is an internationally recognized journal that undergoes a rigorous peer-review process. It focuses on interdisciplinary research related to green energy and the environment, covering a wide range of topics including biofuel and bioenergy, energy storage and networks, catalysis for sustainable processes, and materials for energy and the environment. GEE has a broad scope and encourages the submission of original and innovative research in both fundamental and engineering fields. Additionally, GEE serves as a platform for discussions, summaries, reviews, and previews of the impact of green energy on the eco-environment.