摘要
随着工业化的推进,化石能源的消耗产生大量温室气体,其中CH_(4)和CO_(2)占据温室气体排放的98%以上。将CH_(4)和CO_(2)转化为高附加值化学品具有重要的意义,一直受到工业界和学术界广泛关注。传统的热催化甲烷干重整(DRM)可实现将CH_(4)和CO_(2)转化为合成气,但该反应过程受热力学限制,需要很高的能量输入,并且由于反应温度较高,催化剂易发生积碳而失活。绿色环保的光催化技术可以使甲烷干重整反应在温和条件下进行,但是存在太阳光利用率和反应转化率较低等问题。最近光热协同催化受到学术界广泛关注。许多研究结果表明,在相对温和的条件下,光热催化DRM可以获得良好的催化效果,可有效实现太阳能转化为化学能。本文简要介绍近期光热催化甲烷干重整反应的研究进展,总结不同金属催化剂在光热催化甲烷干重整中的应用,同时提出了光热催化甲烷干重整存在的一些挑战及展望。
During the development of traditional industries,large amounts of greenhouse gases have been emitted due to the increasing consumption of fossil energy.CH_(4)and CO_(2)account for more than 98%of greenhouse gas emissions,and the conversion of CH_(4)and CO_(2)into high value-added chemicals has attracted extensive attention from both industry and academia.Dry reforming of methane(DRM)can co-convert CH_(4)and CO_(2)into syngas,which can be further converted into various value-added fuels and chemicals through Fischer-Tropsch synthesis.The dry reforming of methane into syngas by thermal catalysis provides an effective strategy for the consumption of both CH_(4)and CO_(2),which is beneficial for alleviating environmental problems such as global warming.However,a high-intensity energy input is needed at high temperatures owing to the thermodynamic limitations of the DRM reaction and catalyst instability caused by coke formation.Environmentally friendly photocatalytic technology can make the DRM reaction proceed under mild conditions.However,its development is greatly restricted owing to the low utilization rate of sunlight and low reaction conversion rate.Recently,photothermocatalysis has been widely used in various fields.Many studies have shown that under relatively mild conditions,photothermocatalysis of DRM can achieve promising catalytic performance and effectively convert solar energy into chemical energy.Photothermocatalysis can greatly increase the reaction rate of photocatalytic DRM without a high energy input.In addition,the introduction of light is beneficial for the thermal catalysis of DRM by reducing the reaction activation energy,inhibiting coke formation,and reversing the water-gas shift reaction.In this paper,the advantages and disadvantages of thermal catalysis,photocatalysis,and photothermal catalysis of DRM are first discussed.Then,recent research progress in photothermocatalysis of the DRM reaction,especially the application of different metal-based catalysts(Ni,Pt,Rh,Ru,and Co)is summarized.Localized surface plasmon resonance effects,types of carriers,elimination of coke formation,and suppression of the reverse water-gas shift reaction are briefly mentioned.Finally,the future challenges and new perspectives on the photothermocatalysis of DRM are highlighted,including high utilization of sunlight,catalyst long-term stability,reactor optimization,and the photothermocatalytic mechanism.
作者
何展军
黄敏
林铁军
钟良枢
Zhanjun He;Min Huang;Tiejun Lin;Liangshu Zhong(CAS Key Laboratory of Low-Carbon Conversion Science and Engineering,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China;University of the Chinese Academy of Sciences,Beijing 100049,China;School of Physical Science and Technology,Shanghai Tech University,Shanghai 201210,China)
出处
《物理化学学报》
SCIE
CAS
CSCD
北大核心
2023年第9期22-34,共13页
Acta Physico-Chimica Sinica
基金
国家重点研发计划项目(2021YFF0500702)
上海市自然科学基金项目(22JC1404200)
上海市学术技术带头人项目(20XD1404000)资助。
关键词
甲烷干重整
光热催化
LSPR
金属基催化剂
Dry reforming of methane
Photothermal catalysis
LSPR
Metal-based catalysts
