高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (7): 1600-1608.doi: 10.7503/cjcu20200127

• 物理化学 • 上一篇    下一篇

Pd-Cu/羟磷灰石的制备及常温常湿CO催化氧化性能

李潇1,2,邢莉莎1,2,赵婉君1,2,王永钊1,*(),赵永祥1,*()   

  1. 1.山西大学精细化学品教育部工程研究中心, 太原 030006
    2.山西大学化学化工学院, 太原 030006
  • 收稿日期:2020-03-09 出版日期:2020-07-10 发布日期:2020-04-15
  • 通讯作者: 王永钊,赵永祥 E-mail:catalyst@sxu.edu.cn;yxzhao@sxu.edu.cn
  • 基金资助:
    国家自然科学基金(U1710221);山西省自然科学基金(201801D121043)

Preparation and Characterization of Pd-Cu/hydroxyapatite Catalyst and Its Catalytic Performance for Room-temperature CO Oxidation in Humid Circumstances

LI Xiao1,2,XING Lisha1,2,ZHAO Wanjun1,2,WANG Yongzhao1,*(),ZHAO Yongxiang1,*()   

  1. 1. Engineering Research Center of Ministry of Education for Fine Chemicals, Taiyuan 030006, China
    2. School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China
  • Received:2020-03-09 Online:2020-07-10 Published:2020-04-15
  • Contact: Yongzhao WANG,Yongxiang ZHAO E-mail:catalyst@sxu.edu.cn;yxzhao@sxu.edu.cn
  • Supported by:
    † National Natural Science Foundation of China(U1710221);Natural Science Foundation of Shanxi Province, China(201801D121043)

摘要:

通过溶胶-凝胶法(SG)和水热法(HT)合成了羟磷灰石载体(HAP-SG, HAP-HT), 以浸渍法制备负载型Pd-Cu/HAP催化剂(PC-SG, PC-HT), 并考察其常温常湿条件下CO催化氧化反应性能. 采用电感耦合等离子体发射光谱(ICP-OES)、 N2物理吸附-脱附、 X射线衍射(XRD)、 傅里叶变换红外光谱(FTIR)、 H2程序升温还原(H2-TPR)、 CO2程序升温脱附(CO2-TPD)、 X射线光电子能谱(XPS)和CO原位漫反射傅里叶变换红外光谱(in-situ DRIFTS)等手段对Pd-Cu/HAP催化剂进行了表征. 结果表明, 相比于PC-SG, PC-HT具有较大比表面积和孔容, 含有较多的Cu2Cl(OH)3物种且与Pd物种和载体直接产生了较强的相互作用; 而且PC-HT表面含有较强CO活化能力的Pd+物种和更多具有较强氧化还原性质的Cu+物种, 以及较少数量和较低强度的碱性位点, 因而表现出更加优异的常温常湿条件下CO催化氧化性能.

关键词: 钯-铜/羟磷灰石, 常温常湿, 一氧化碳催化氧化, 氧化还原, 钯离子物种

Abstract:

Hydroxyapatite supports(HAP-SG, HAP-HT) were prepared by sol-gel and hydrothermal methods, respectively. Pd-Cu/HAP catalysts(PC-SG, PC-HT) were synthesized by an impregnation method, and the catalytic activities toward CO oxidation at room temperature and in humid circumstances were investigated. The Pd-Cu/HAP catalysts were characterized by inductively coupled plasma optical emission spectrometry(ICP-OES), N2-physisorption, X-ray diffraction(XRD), Fourier transform infrared(FTIR), H2 temperature programmed reduction(H2-TPR), CO2 temperature programmed desorption(CO2-TPD), X-ray photoelectron spectroscopy(XPS)and CO in-situ diffuse reflection using Fourier transform spectroscopy(DRIFTS). The results show that compared with PC-SG, PC-HT possesses the larger specific surface area and pore volume, contains more Cu2Cl(OH)3 species with stronger interactions with Pd species and support; more importantly, Pd+ species with stronger CO activation ability and more Cu+ species with stronger redox property, as well as fewer and weaker basic sites present in PC-HT, thus PC-HT exhibits more excellent CO catalytic oxidation performance for room-temperature CO oxidation in humid circumstances.

Key words: Pd-Cu/hydroxyapatite, Room temperature and in humid circumstances, CO catalytic oxidation, Redox, Pd+ species

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