摘要
为实现碳达峰、碳中和目标,除加大节能减排力度之外,还需进一步加强对CO_(2)、CH_(4)等温室气体的资源化利用,甲烷干重整(DRM)利用CO_(2)和CH_(4)生产H_(2)和CO合成气是一个备受关注的热点。采用“双溶剂”法制备纳米片、纳米棒和纳米颗粒三种形貌γ-Al_(2)O_(3)载体,研究了载体形貌对Ni/γ-Al_(2)O_(3)催化DRM的影响。结果表明,Ni/Al_(2)O_(3)活性受γ-Al_(2)O_(3)载体形貌影响,Ni负载于Al_(2)O_(3)纳米棒催化剂表现出优异的活性,CO_(2)和CH_(4)的初始转化率分别是84.3%和75.4%,产物中H_(2)/CO的比例为0.88,在反应过程中稳定性最高,没有失活迹象,与Ni负载于市售Al_(2)O_(3)催化剂相比,CO_(2)和CH_(4)的转化率提升23.6和26.8个百分点。这是由于高比表面积的Ni负载于Al_(2)O_(3)纳米棒催化剂有利于Ni金属在表面的分散,存在较多的Ni的活性位点抑制反应过程中的Ni颗粒的团聚;Ni负载于Al_(2)O_(3)纳米棒催化剂拥有最多的碱性位点,有利于CO_(2)在催化剂表面的吸附活化。
To achieve the goal of emission peak and carbon neutrality,in addition to increasing energy savings and emission reduction,it is necessary to further strengthen the utilization of greenhouse gases such as CO_(2) and CH_(4).Dry reforming of methane(DRM)to produce H_(2) and CO syngas from CO_(2) and CH_(4) is a hot topic of interest.γ-Al_(2)O_(3) supports with morphologies of nano-rod,nanosheet,and nano particle were prepared by a“two-solvent”method,and the effect of support morphologies on Ni/γ-Al_(2)O_(3) catalyzed DRM was investigated.The results showed that the Ni/γ-Al_(2)O_(3) activity was influenced by the morphology of theγ-Al_(2)O_(3) support,and Ni supported on nano-rod Al_(2)O_(3) exhibited excellent activity with initial conversions of 84.3%and 75.4%for CO_(2) and CH_(4),respectively,and R H2/CO of 0.88 in syngas,with the highest stability during the reaction and no signs of deactivation.Compared with Ni supported on commercial Al_(2)O_(3) catalysts,CO_(2) and CH_(4) conversions were increased by 23.6 and 26.8 percentage points,respectively.This is due to the high specific surface area of Ni supported on nano-rod Al_(2)O_(3) catalysts,which facilitates the dispersion of Ni metal on the surface and the presence of more active sites of Ni to inhibit the agglomeration of Ni particles during the reaction;Ni supported on nano-rod Al_(2)O_(3) exhibits the highest number of basic sites,which facilitates the activation of CO_(2) adsorption on the catalyst surface.
作者
王传棽
苏通明
秦祖赠
纪红兵
Wang Chuanshen;Su Tongming;Qin Zuzeng;Ji Hongbing(Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology,School of Chemistry and Chemical Engineering,Guangxi University,Nanning 530004,Guangxi,China;School of Chemistry,Sun Yat-Sen University,Guangzhou 510275,Guangdong,China)
出处
《工业催化》
CAS
2022年第11期31-42,共12页
Industrial Catalysis
基金
国家自然科学基金项目(22078074)
广西自然科学基金项目(2020GXNSFDA297007)
广西石化资源加工及过程强化技术重点实验室开放项目(2020K002)
广西八桂学者专项基金。