Ni-Co双金属催化剂上沼气重整制氢机理

引用本文: 徐军科, 沈利红, 周伟, 马建新. Ni-Co双金属催化剂上沼气重整制氢机理[J]. 物理化学学报, 2011, 27(03): 697-704. doi: 10.3866/PKU.WHXB20110309 shu

Citation: XU Jun-Ke, SHEN Li-Hong, ZHOU Wei, MA Jian-Xin. Mechanism of Biogas Reforming for Hydrogen Production over Ni-Co Bimetallic Catalyst[J]. Acta Physico-Chimica Sinica, 2011, 27(03): 697-704. doi: 10.3866/PKU.WHXB20110309 shu

Ni-Co双金属催化剂上沼气重整制氢机理

基金项目:
科技部国际合作重点项目(2007DFC61690) (2007DFC61690)

汉高同济教席(081591)资助 (081591)

摘要:

用传统湿式浸渍法制备了La₂O₃掺杂的商业γ-Al₂O₃负载的沼气重整催化剂Ni-Co/La₂O₃-γ-Al₂O₃, 并用程序升温加氢(TPH)、程序升温氧化(TPO)、程序升温表面反应(TPSR)、程序升温脱附(TPD)及脉冲实验对催化剂进行了表征. 结果表明, 沼气重整过程中Ni-Co/La₂O₃-γ-Al₂O₃催化剂上的表面碳物种主要来源于CH₄的裂解, CO₂的贡献很小. CH₄裂解能够产生三种活性不同的碳物种, 即C_α、C_β与C_γ. 随着反应的进行, C_α物种减小而C_β与C_γ物种增加, 且C_γ物种能够转变为惰性的石墨碳. 重整反应过程中CH₄与CO₂的活化能相互促进. 催化剂表面的O物种与C反应生成CO或与CH_x反应生成CH_xO再分解为CO与吸附态的H物种, 可能是Ni-Co/La₂O₃-γ-Al₂O₃催化剂上沼气重整的速率控制步骤.

关键词:

镍
/ 钴
/ 双金属催化剂
/ 沼气重整
/ 制氢
/ 机理

English

Mechanism of Biogas Reforming for Hydrogen Production over Ni-Co Bimetallic Catalyst

1.
1. Clean Energy Automotive Engineering Center, Tongji University, Shanghai 201804, P. R. China;
2. Shanghai Baoshan Environmental Monitoring Station, Shanghai 201901, P. R. China;
3. School of Automotive Engineering, Tongji University, Shanghai 201804, P. R. China
Received Date: 27 September 2010
Available Online: 03 March 2011
Fund Project:
科技部国际合作重点项目(2007DFC61690)

汉高同济教席(081591)资助

Abstract:

Ni-Co bimetallic catalysts supported on commercial γ-Al₂O₃ modified with La₂O₃ were prepared by conventional incipient wetness impregnation for biogas reforming. The catalysts were characterized using temperature-programmed hydrogenation (TPH), temperature-programmed oxygenation (TPO), temperature-programmed surface reaction (TPSR), temperature-programmed desorption (TPD), and a pulse experiment. During biogas reforming the surface carbon species on Ni-Co/La₂O₃-γ-Al₂O₃ originated mainly from the cracking of CH₄ and the contribution of CO₂ was insignificant. Cracking of CH₄ results in three carbon species of C_α, C_β, and C_γ, which have different reaction activities. During the reaction, the amount of C_α decreased but C_β and C_γ increased. In addition, C_γ could be changed into inactive graphite carbon. The activation of CH₄ and CO₂ was mutually promoted in the reforming reaction. It was revealed that the controlling step for biogas reforming over the Ni-Co/La₂O₃-γ-Al₂O₃ catalyst could be the reaction of the surface species of O with C to form CO or with CH_x to give CH_xO followed by the formation of CO and adsorbed H.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

Ni-Co双金属催化剂上沼气重整制氢机理

English

Mechanism of Biogas Reforming for Hydrogen Production over Ni-Co Bimetallic Catalyst

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Ni-Co双金属催化剂上沼气重整制氢机理

English

Mechanism of Biogas Reforming for Hydrogen Production over Ni-Co Bimetallic Catalyst

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

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CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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