全球变暖的问题正变得日益严峻,碳减排碳中和已成为国际社会的共识和努力目标。作为CO_(2)减排的重要方式之一,二氧化碳捕集、利用与封存(Carbon Capture,Utilization and Storage,CCUS)近年来备受关注并且发展迅猛。CO_(2)海洋封存作...全球变暖的问题正变得日益严峻,碳减排碳中和已成为国际社会的共识和努力目标。作为CO_(2)减排的重要方式之一,二氧化碳捕集、利用与封存(Carbon Capture,Utilization and Storage,CCUS)近年来备受关注并且发展迅猛。CO_(2)海洋封存作为其中一种最具潜力的减排方式,了解其发展现状对进一步研究CO_(2)封存具有重要的参考价值。本文介绍了CO_(2)海洋封存的方法和封存机理,总结了该技术在国内外研究进展。此外,文章还概述了我国在CO_(2)海洋封存上的巨大潜力和库源匹配上的优势,以及海洋封存对环境可能造成的影响。最后,指出推进CO_(2)海洋封存技术的研究并开发相应的能力,将有助于加速推进碳减排进程、尽快实现碳中和目标。展开更多
随着全球工业化进程加快,大量二氧化碳被快速地排放到大气中,产生诸多环境问题。CO_(2)作为一种重要的碳资源,通过加氢制备高附加值化学品近年来逐渐受到研究人员广泛关注。芳烃作为一种基本化工原料,传统上主要靠石油裂解和石脑油重整...随着全球工业化进程加快,大量二氧化碳被快速地排放到大气中,产生诸多环境问题。CO_(2)作为一种重要的碳资源,通过加氢制备高附加值化学品近年来逐渐受到研究人员广泛关注。芳烃作为一种基本化工原料,传统上主要靠石油裂解和石脑油重整来生产,通过CO_(2)加氢制备芳烃可以有效减缓对化石能源的过度依赖。但是CO_(2)的惰性强、活化能垒高、C–C偶联精准调控难,使低温CO_(2)加氢制备芳烃的高效催化剂开发存在巨大挑战。目前,采用氧化物–分子筛复合催化剂体系可以将CO_(2)加氢合成甲醇与甲醇制芳烃反应进行耦合,实现CO_(2)加氢直接合成芳烃。本文通过共沉淀法制备了ZnZrO_(x)复合氧化物,并采用等体积浸渍法引入不同过渡金属(Fe、Cu、Co、Ni),随后将其与商用ZSM-5分子筛物理混合制备了M-ZnZrO_(x)/ZSM-5复合催化剂。在275℃、H_(2)/CO_(2)=3、空速为600 m L/(g·h)的反应条件下,采用质量分数为4%的Fe改性的Fe-ZnZrO_(x)与ZSM-5组成的复合催化剂,芳烃选择性高达80.4%,CO_(2)转化率为5.6%,CO选择性为42.2%。进一步探究了ZnZrO_(x)氧化物上Fe含量对复合催化剂性能的影响,发现Fe含量增加有助于提升反应活性与芳烃选择性;当Fe负载量为8%时,芳烃选择性提升至85.0%。这一研究为在温和条件下通过CO_(2)加氢制备芳烃工业催化剂的开发提供了新思路。展开更多
Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by...Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by varying the calcination temperature of anatase-TiO_(2).Structural characterizations revealed that a distinct TiO_(x) coating on the Ni nanoparticles(NPs)was evident for Ni/TiO_(2)-700 catalyst due to strong metal-support interaction.It is observed that the TiOx overlayer gradually disappeared as the ratio of rutile/anatase increased,thereby enhancing the exposure of Ni active sites.The exposed Ni sites enhanced visible light absorption and boosted the dissociation capability of CH4,which led to the much elevated catalytic activity for Ni/TiO_(2)-950 in which rutile dominated.Therefore,the catalytic activity of solar-driven DRM reaction was significantly influenced by the rutile/anatase ratio.Ni/TiO_(2)-950,characterized by a predominant rutile phase,exhibited the highest DRM reactivity,with remarkable H_(2) and CO production rates reaching as high as 87.4 and 220.2 mmol/(g·h),respectively.These rates were approximately 257 and 130 times higher,respectively,compared to those obtained on Ni/TiO_(2)-700 with anatase.This study suggests that the optimization of crystal structure of TiO_(2) support can effectively enhance the performance of photothermal DRM reaction.展开更多
文摘全球变暖的问题正变得日益严峻,碳减排碳中和已成为国际社会的共识和努力目标。作为CO_(2)减排的重要方式之一,二氧化碳捕集、利用与封存(Carbon Capture,Utilization and Storage,CCUS)近年来备受关注并且发展迅猛。CO_(2)海洋封存作为其中一种最具潜力的减排方式,了解其发展现状对进一步研究CO_(2)封存具有重要的参考价值。本文介绍了CO_(2)海洋封存的方法和封存机理,总结了该技术在国内外研究进展。此外,文章还概述了我国在CO_(2)海洋封存上的巨大潜力和库源匹配上的优势,以及海洋封存对环境可能造成的影响。最后,指出推进CO_(2)海洋封存技术的研究并开发相应的能力,将有助于加速推进碳减排进程、尽快实现碳中和目标。
文摘随着全球工业化进程加快,大量二氧化碳被快速地排放到大气中,产生诸多环境问题。CO_(2)作为一种重要的碳资源,通过加氢制备高附加值化学品近年来逐渐受到研究人员广泛关注。芳烃作为一种基本化工原料,传统上主要靠石油裂解和石脑油重整来生产,通过CO_(2)加氢制备芳烃可以有效减缓对化石能源的过度依赖。但是CO_(2)的惰性强、活化能垒高、C–C偶联精准调控难,使低温CO_(2)加氢制备芳烃的高效催化剂开发存在巨大挑战。目前,采用氧化物–分子筛复合催化剂体系可以将CO_(2)加氢合成甲醇与甲醇制芳烃反应进行耦合,实现CO_(2)加氢直接合成芳烃。本文通过共沉淀法制备了ZnZrO_(x)复合氧化物,并采用等体积浸渍法引入不同过渡金属(Fe、Cu、Co、Ni),随后将其与商用ZSM-5分子筛物理混合制备了M-ZnZrO_(x)/ZSM-5复合催化剂。在275℃、H_(2)/CO_(2)=3、空速为600 m L/(g·h)的反应条件下,采用质量分数为4%的Fe改性的Fe-ZnZrO_(x)与ZSM-5组成的复合催化剂,芳烃选择性高达80.4%,CO_(2)转化率为5.6%,CO选择性为42.2%。进一步探究了ZnZrO_(x)氧化物上Fe含量对复合催化剂性能的影响,发现Fe含量增加有助于提升反应活性与芳烃选择性;当Fe负载量为8%时,芳烃选择性提升至85.0%。这一研究为在温和条件下通过CO_(2)加氢制备芳烃工业催化剂的开发提供了新思路。
基金The project was supported by Natural Science Foundation of China(22072177)Natural Science Foundation of Shanghai(21ZR1471700)Shanghai Youth Science and Technology Talents Sailing Program(21YF1453600)。
基金The project was supported by the National Key R&D Program of China(2021YFF0500702)Natural Science Foundation of Shanghai(22JC1404200)+3 种基金Program of Shanghai Academic/Technology Research Leader(20XD1404000)Natural Science Foundation of China(U22B20136,22293023)Science and Technology Major Project of Inner Mongolia(2021ZD0042)the Youth Innovation Promotion Association of CAS。
文摘Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by varying the calcination temperature of anatase-TiO_(2).Structural characterizations revealed that a distinct TiO_(x) coating on the Ni nanoparticles(NPs)was evident for Ni/TiO_(2)-700 catalyst due to strong metal-support interaction.It is observed that the TiOx overlayer gradually disappeared as the ratio of rutile/anatase increased,thereby enhancing the exposure of Ni active sites.The exposed Ni sites enhanced visible light absorption and boosted the dissociation capability of CH4,which led to the much elevated catalytic activity for Ni/TiO_(2)-950 in which rutile dominated.Therefore,the catalytic activity of solar-driven DRM reaction was significantly influenced by the rutile/anatase ratio.Ni/TiO_(2)-950,characterized by a predominant rutile phase,exhibited the highest DRM reactivity,with remarkable H_(2) and CO production rates reaching as high as 87.4 and 220.2 mmol/(g·h),respectively.These rates were approximately 257 and 130 times higher,respectively,compared to those obtained on Ni/TiO_(2)-700 with anatase.This study suggests that the optimization of crystal structure of TiO_(2) support can effectively enhance the performance of photothermal DRM reaction.
