无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ
催化材料

Zn/Co-ZIF衍生多孔碳钯基催化剂的制备及在甲酸制氢中的应用

  • 刘青翠 ,
  • 李云青 ,
  • 庞瑞琪 ,
  • 田亚萍 ,
  • 陈一莹 ,
  • 李芳 ,
  • 李其明
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  • 辽宁石油化工大学石油化工学院,辽宁 抚顺 113001
刘青翠(1998— ),女,硕士,研究方向为催化材料及储氢能源;E-mail:2675329910@qq.com
李芳(1978— ),女,副教授,硕士生导师;E-mail:lflamp@163.com
李其明(1977— ),男,教授,研究方向为催化材料及储氢能源;E-mail:lqm_dicp@163.com

收稿日期: 2023-10-30

  网络出版日期: 2024-06-20

基金资助

国家自然科学基金项目(21703091);辽宁省教育厅资助项目(LJKMZ20220724);辽宁省教育厅资助项目(JYTMS20231442)

Preparation of Zn/Co-ZIF derived porous carbon supported Pd as catalyst and its application to formic acid dehydrogenation

  • LIU Qingcui ,
  • LI Yunqing ,
  • PANG Ruiqi ,
  • TIAN Yaping ,
  • CHEN Yiying ,
  • LI Fang ,
  • LI Qiming
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  • School of Chemical Engineering,Liaoning Petrochemical University,Fushun 113001,China

Received date: 2023-10-30

  Online published: 2024-06-20

摘要

通过浸渍还原法将Pd、Ag等锚定在经过HNO3酸化和(NH42HPO4磷化处理得到的Zn/Co-ZIF衍生HPNC多孔碳上,制备出高活性的Ag1Pd7@HPNC催化剂。采用XRD、TEM、SEM和EDS等系列表征手段对Zn/Co-ZIF、多孔碳载体和制备的催化剂进行了表征分析和系统测试。结果表明,多孔碳中的Zn和大部分的Co物种可通过高温焙烧和酸化处理方式被有效去除,小尺寸的Pd和Ag纳米颗粒可高效负载于HPNC多孔碳载体的表面。通过探究不同载体及银钯不同的质量比对催化剂催化活性的影响,证明了Ag1Pd7@HPNC催化剂具有优异的甲酸催化性能。甲酸分解实验表明,经(NH42HPO4处理后的Pd@HPNC催化剂活性优于未处理的Pd@HNC催化剂活性。掺杂Ag会进一步提高Ag x Pd y @HPNC(x>0)双金属催化剂的催化活性,其中当mAgmPd=1∶7时,Ag1Pd7@HPNC催化甲酸分解活性最佳,在318 K条件下甲酸分解的转化频率(TOF)可达1 025 h-1;并且该催化剂循环使用5次后TOF仍保持为920 h-1,表明其具有良好的循环稳定性。Ag1Pd7@HPNC在甲酸催化脱氢方面展示了较好的应用前景。

本文引用格式

刘青翠 , 李云青 , 庞瑞琪 , 田亚萍 , 陈一莹 , 李芳 , 李其明 . Zn/Co-ZIF衍生多孔碳钯基催化剂的制备及在甲酸制氢中的应用[J]. 无机盐工业, 2024 , 56(6) : 147 -152 . DOI: 10.19964/j.issn.1006-4990.2023-0517

Abstract

Highly active Ag1Pd7@HPNC catalyst were obtained through anchoring Ag and Pd on Zn/Co-ZIF derived nitrogen-doped porous carbon(HPNC),which was obtained by HNO3 immersion and(NH42HPO4 phosphating.Zn/Co-ZIF,porous carbon supports and prepared catalysts were characterized and systematically analyzed by a series of characterization methods such as XRD,TEM,SEM and EDS,etc.The results showed that Zn and most of Co species in porous carbon could be effectively removed by high-temperature sintering and acidification treatment,and small-size Pd and Ag nanoparticles could be efficiently loaded on the surface of HPNC porous carbon carriers.By exploring the effects of different catalyst supports and different mAgmPd on the catalyst catalysts,it was demonstrated that the Ag1Pd7@HPNC catalysts had excellent formic acid catalytic activity.The formic acid dehydrogenation experiment showed that the catalytic activity of Pd@HPNC treated by(NH42HPO4 was superior to that of untreated Pd@HNC catalyst,and the catalytic activity of Ag x Pd y @HPNC (x>0) prepared by doping Ag species had been further improved.When the mass ratio of mAgmPd=1∶7,the catalytic activity of Ag1Pd7@HPNC for formic acid decomposition was optimal with a turnover frequency(TOF) of 1 025 h-1 for formic acid at 318 K,and the catalyst was recycled for five times with the TOF value of 920 h-1,indicating its good recycling stability.Ag1Pd7@HPNC showed a good application prospect to formic acid dehydrogenation.

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