物理化学学报 >> 1998, Vol. 14 >> Issue (08): 737-741.doi: 10.3866/PKU.WHXB19980813

研究论文 上一篇    下一篇

甲烷部分氧化Ni催化剂及助剂的研究

金荣超, 陈燕馨, 李文钊, 季亚英, 秦永生, 江义   

  1. 中国科学院大连化学物理研究所，大连 116023
  • 收稿日期:1997-11-18 修回日期:1998-03-20 发布日期:1998-08-15
  • 通讯作者: 金荣超

Ni/α-Al2O3 Catalyst for the Partial Oxidation of Methane to Syngas

Jin Rong-Chao, Chen Yan-Xin, Li Wen-Zhao, Ji Ya-Ying, Qin Yong-Sheng, Jiang Yi   

  1. Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023
  • Received:1997-11-18 Revised:1998-03-20 Published:1998-08-15
  • Contact: Jin Rong-Chao

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摘要：

考察了不同Ni担载量的Ni／a－Al_2O_3催化剂的催化性能，以8％Ni（质量分数）最佳．XRD分析表明，8％Ni催化剂表面NiO颗粒最小．TPR分析表明，催化剂表面主要有两种不同化学环境的NiO，当Ni担载量超过12％时，表面开始出现“游离态”NiO，这部分NiO易使催化剂积碳．添加稀土Ce有利于提高Ni催化剂的活性、选择性和稳定性，并对Ce的助剂效应作了研究．

关键词: 甲烷, 氧化, Ni催化剂, 助剂

Abstract:

The catalytic performance of Ni/α-Al2O3 catalysts with different nickel content was investigated for the partial oxidation of methane to syngas in O2 at atmospheric pressure and very high space velecity of 5×105h-1. Optimal CH4 conversion of 91%, CO and H2 selectivity of 94%and 96%, respectively were obtained over 8%(mass fraction) N1 catalyst at 800 ℃, XRD (X-ray Diffraction) analysis indicated that oxidic nickel is the main surface species on Ni/α-Al2O3 catalyst calcinated at 800℃ under atmosphere. TPR (Temperature Programmed Reduction) suggested a bimodel nature of oxidic nickel that are "fixed" to the support. The "free" oxidie nickel, which is responsible for the serious carbon deposition on catalyst, appeared as the nickel content was increased up to 12%. Promoter effects of lanthanide oxide (CeO2) were also investigated. The results showed that addition of CeO2 was beneficial to CH4 conversion and CO selectivity. An excellant conversion (96.5%) and CO selection (96%) were achieved on NiCe(1%Ce)/α-Al2O3 at 800 ℃ with a space velecity of 5×105h-1. Furthmore, CeO2 significantly improved the stability of nickel under critical reaction conditions. No carbon deposition was found over NiCe(1%Ce)/α-Al2O3 after nine hours at 900℃. The promoting mechanism of CeO2 was discussed on the basis of XPS, TPR and XRD results.

Key words: Methane, Syngas, Nickel, Promoter