Smita Takawane, Masatoshi Miyamoto, Takumi Watanabe and Tomonori Ohba
{"title":"钛酸钡纳米催化剂上随压力变化的二氧化碳热解作用","authors":"Smita Takawane, Masatoshi Miyamoto, Takumi Watanabe and Tomonori Ohba","doi":"10.1039/D4SU00253A","DOIUrl":null,"url":null,"abstract":"<p >Rising CO<small><sub>2</sub></small> levels pose a significant threat to global warming, extreme weather events, and ecosystem disruption. Mitigating these effects requires a reduction in CO<small><sub>2</sub></small> concentration using innovative technologies for CO<small><sub>2</sub></small> capture, storage, and utilization. Perovskite-type barium titanate nanocatalysts have the potential for high CO<small><sub>2</sub></small> conversion into valuable solid carbon products at low temperatures. In this study, we investigated the pressure-dependent CO<small><sub>2</sub></small> conversion activity of barium titanate nanocatalysts at 700 K. A key focus of this study is the impact of pressure on the interaction between CO<small><sub>2</sub></small> molecules and barium titanate nanocatalysts to evaluate the CO<small><sub>2</sub></small> conversion mechanism. The primary structures of the nanocatalysts remained unchanged after CO<small><sub>2</sub></small> thermolysis, whereas carbon was deposited on the nanocatalysts above 0.05 MPa. The reactant carbons after CO<small><sub>2</sub></small> conversion at various pressures between 0.01 and 1.0 MPa at 700 K were evaluated by temperature-programmed desorption in an O<small><sub>2</sub></small> atmosphere. The desorption peaks observed at approximately 500 K, 800–900 K, and 900–1300 K were the results of desorption of chemisorbed CO<small><sub>2</sub></small>, less- and high-crystalline graphitic carbons. Chemisorbed CO<small><sub>2</sub></small> and less-crystalline graphitic carbon were observed at 0.05 MPa. Highly crystalline graphitic carbons were observed on the nanocatalysts after CO<small><sub>2</sub></small> thermolysis at 0.1–1.0 MPa as well as chemisorbed CO<small><sub>2</sub></small>, although the amount of carbon at 1.0 MPa was smaller than the others. Therefore, the approach of CO<small><sub>2</sub></small> thermolysis at a low temperature of 700 K and 0.1–0.5 MPa is promising for producing valuable solid carbon products and mitigating the environmental impact of CO<small><sub>2</sub></small> emissions.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00253a?page=search","citationCount":"0","resultStr":"{\"title\":\"Pressure-dependent CO2 thermolysis on barium titanate nanocatalysts†\",\"authors\":\"Smita Takawane, Masatoshi Miyamoto, Takumi Watanabe and Tomonori Ohba\",\"doi\":\"10.1039/D4SU00253A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Rising CO<small><sub>2</sub></small> levels pose a significant threat to global warming, extreme weather events, and ecosystem disruption. 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The reactant carbons after CO<small><sub>2</sub></small> conversion at various pressures between 0.01 and 1.0 MPa at 700 K were evaluated by temperature-programmed desorption in an O<small><sub>2</sub></small> atmosphere. The desorption peaks observed at approximately 500 K, 800–900 K, and 900–1300 K were the results of desorption of chemisorbed CO<small><sub>2</sub></small>, less- and high-crystalline graphitic carbons. Chemisorbed CO<small><sub>2</sub></small> and less-crystalline graphitic carbon were observed at 0.05 MPa. Highly crystalline graphitic carbons were observed on the nanocatalysts after CO<small><sub>2</sub></small> thermolysis at 0.1–1.0 MPa as well as chemisorbed CO<small><sub>2</sub></small>, although the amount of carbon at 1.0 MPa was smaller than the others. 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引用次数: 0
摘要
二氧化碳浓度的上升对全球变暖、极端天气事件和生态系统破坏构成了重大威胁。要减轻这些影响,就必须利用二氧化碳捕获、储存和利用的创新技术降低二氧化碳浓度。包晶型钛酸钡纳米催化剂具有在低温条件下将二氧化碳转化为有价值的固态碳产品的潜力。本研究的重点是压力对二氧化碳分子与钛酸钡纳米催化剂之间相互作用的影响,从而评估二氧化碳的转化机理。二氧化碳热解后,纳米催化剂的主要结构保持不变,而碳则沉积在 0.05 兆帕以上的纳米催化剂上。在 700 K 条件下,在 0.01 至 1.0 MPa 的不同压力下进行二氧化碳转化后的反应物碳通过在氧气环境中的温度编程解吸进行了评估。在大约 500 K、800-900 K 和 900-1300 K 处观察到的解吸峰是化学吸附二氧化碳、少晶和高晶石墨碳解吸的结果。在 0.05 兆帕时可观察到化学吸附的二氧化碳和少晶石墨碳。在 0.1-1.0 兆帕的二氧化碳热解条件下,纳米催化剂上观察到了高结晶石墨碳以及化学吸附的二氧化碳,但 1.0 兆帕时的碳量比其他条件下的碳量少。因此,在 700 K 低温和 0.1-0.5 MPa 下进行二氧化碳热解的方法有望生产出有价值的固体碳产品,并减轻二氧化碳排放对环境的影响。
Pressure-dependent CO2 thermolysis on barium titanate nanocatalysts†
Rising CO2 levels pose a significant threat to global warming, extreme weather events, and ecosystem disruption. Mitigating these effects requires a reduction in CO2 concentration using innovative technologies for CO2 capture, storage, and utilization. Perovskite-type barium titanate nanocatalysts have the potential for high CO2 conversion into valuable solid carbon products at low temperatures. In this study, we investigated the pressure-dependent CO2 conversion activity of barium titanate nanocatalysts at 700 K. A key focus of this study is the impact of pressure on the interaction between CO2 molecules and barium titanate nanocatalysts to evaluate the CO2 conversion mechanism. The primary structures of the nanocatalysts remained unchanged after CO2 thermolysis, whereas carbon was deposited on the nanocatalysts above 0.05 MPa. The reactant carbons after CO2 conversion at various pressures between 0.01 and 1.0 MPa at 700 K were evaluated by temperature-programmed desorption in an O2 atmosphere. The desorption peaks observed at approximately 500 K, 800–900 K, and 900–1300 K were the results of desorption of chemisorbed CO2, less- and high-crystalline graphitic carbons. Chemisorbed CO2 and less-crystalline graphitic carbon were observed at 0.05 MPa. Highly crystalline graphitic carbons were observed on the nanocatalysts after CO2 thermolysis at 0.1–1.0 MPa as well as chemisorbed CO2, although the amount of carbon at 1.0 MPa was smaller than the others. Therefore, the approach of CO2 thermolysis at a low temperature of 700 K and 0.1–0.5 MPa is promising for producing valuable solid carbon products and mitigating the environmental impact of CO2 emissions.