{"title":"自下而上合理合成用于单原子铂催化剂载体的富硫多孔碳","authors":"Koki Chida, Takeharu Yoshii, Ryo Kawaguchi, Masataka Inoue, Fumito Tani, Tatsuki Sobue, Shunsuke Ohtani, Kenichi Kato, Tomoki Ogoshi, Shoko Nakahata, Kazuhide Kamiya and Hirotomo Nishihara","doi":"10.1039/D4GC02055C","DOIUrl":null,"url":null,"abstract":"<p >Single-atomic metal catalysts are attractive for green chemistry in terms of their outstanding catalytic performance and savings in precious metal usage owing to maximized metal utilization, including anode catalysts in polymer electrolyte fuel cells (PEFCs). Heteroatom-doped porous carbons are extensively used as supports, where the heteroatoms contribute to the immobilization of single-atomic metals. However, high-content doping of heteroatoms, especially sulphur (S), into carbon supports is still challenging because S species can be readily desorbed during heat treatment. Herein, we present a bottom-up fabrication approach for S-rich porous carbons from molecular precursors <em>via</em> a thermal polymerization process. A simple carbonization of molecules with thermally stable S-containing building blocks and polymerizable ethynyl moieties at 900 °C yields microporous carbon materials with record-high S content (over 15 wt%). The abundant S species function as an effective anchoring site for single-atomic platinum (Pt) species. Toward anode catalysts in PEFCs, the prepared single-atomic Pt catalysts efficiently promote the electrochemical hydrogen oxidation reaction, whose activity is comparable to that of commercial Pt/C, despite the significantly low Pt loading amount.</p>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc02055c?page=search","citationCount":"0","resultStr":"{\"title\":\"Rational bottom-up synthesis of sulphur-rich porous carbons for single-atomic platinum catalyst supports†\",\"authors\":\"Koki Chida, Takeharu Yoshii, Ryo Kawaguchi, Masataka Inoue, Fumito Tani, Tatsuki Sobue, Shunsuke Ohtani, Kenichi Kato, Tomoki Ogoshi, Shoko Nakahata, Kazuhide Kamiya and Hirotomo Nishihara\",\"doi\":\"10.1039/D4GC02055C\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Single-atomic metal catalysts are attractive for green chemistry in terms of their outstanding catalytic performance and savings in precious metal usage owing to maximized metal utilization, including anode catalysts in polymer electrolyte fuel cells (PEFCs). Heteroatom-doped porous carbons are extensively used as supports, where the heteroatoms contribute to the immobilization of single-atomic metals. However, high-content doping of heteroatoms, especially sulphur (S), into carbon supports is still challenging because S species can be readily desorbed during heat treatment. Herein, we present a bottom-up fabrication approach for S-rich porous carbons from molecular precursors <em>via</em> a thermal polymerization process. A simple carbonization of molecules with thermally stable S-containing building blocks and polymerizable ethynyl moieties at 900 °C yields microporous carbon materials with record-high S content (over 15 wt%). The abundant S species function as an effective anchoring site for single-atomic platinum (Pt) species. Toward anode catalysts in PEFCs, the prepared single-atomic Pt catalysts efficiently promote the electrochemical hydrogen oxidation reaction, whose activity is comparable to that of commercial Pt/C, despite the significantly low Pt loading amount.</p>\",\"PeriodicalId\":78,\"journal\":{\"name\":\"Green Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.3000,\"publicationDate\":\"2024-07-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.rsc.org/en/content/articlepdf/2024/gc/d4gc02055c?page=search\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/gc/d4gc02055c\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/gc/d4gc02055c","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
单原子金属催化剂具有出色的催化性能,并能最大限度地利用金属,从而节省贵金属用量,因此对绿色化学(包括聚合物电解质燃料电池(PEFC)中的阳极催化剂)很有吸引力。掺杂杂原子的多孔碳被广泛用作载体,其中的杂原子有助于固定单原子金属。然而,将杂质原子(尤其是硫(S))高含量掺杂到碳支撑物中仍然具有挑战性,因为 S 物种在热处理过程中很容易被解吸。在此,我们提出了一种自下而上的方法,通过热聚合工艺,利用分子前驱体制造富含 S 的多孔碳。在 900 °C 的温度下,对具有热稳定含 S 构建块和可聚合乙炔基的分子进行简单的碳化处理,就能得到 S 含量创纪录地高(超过 15 wt%)的微孔碳材料。丰富的 S 物质可作为单原子铂 (Pt) 物质的有效锚定位点。作为 PEFCs 的阳极催化剂,所制备的单原子铂催化剂能有效促进电化学氢氧化反应,尽管铂负载量很低,但其活性与商用 Pt/C 相当。
Rational bottom-up synthesis of sulphur-rich porous carbons for single-atomic platinum catalyst supports†
Single-atomic metal catalysts are attractive for green chemistry in terms of their outstanding catalytic performance and savings in precious metal usage owing to maximized metal utilization, including anode catalysts in polymer electrolyte fuel cells (PEFCs). Heteroatom-doped porous carbons are extensively used as supports, where the heteroatoms contribute to the immobilization of single-atomic metals. However, high-content doping of heteroatoms, especially sulphur (S), into carbon supports is still challenging because S species can be readily desorbed during heat treatment. Herein, we present a bottom-up fabrication approach for S-rich porous carbons from molecular precursors via a thermal polymerization process. A simple carbonization of molecules with thermally stable S-containing building blocks and polymerizable ethynyl moieties at 900 °C yields microporous carbon materials with record-high S content (over 15 wt%). The abundant S species function as an effective anchoring site for single-atomic platinum (Pt) species. Toward anode catalysts in PEFCs, the prepared single-atomic Pt catalysts efficiently promote the electrochemical hydrogen oxidation reaction, whose activity is comparable to that of commercial Pt/C, despite the significantly low Pt loading amount.
期刊介绍:
Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.