坑洞缺陷限域的金属亚纳米簇用于异相催化
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- 英文论文题名：Pit-type Defects Confined Metal Clusters for Heterogeneous catalysis
- 论文作者：陈少卿 ; 李莉萍 ; 黄新松 ; 李慧霞 ; 李广社
- 英文论文作者：Shaoqing Chen ; Liping Li ; Xinsong Huang ; Huixia Li ; Guangshe Li ; Fujian Institute of Research on the Structure of Matter ; CAS ; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry ; College of Chemistry ; Jilin University
- 年：2016
- 作者机构：中国科学院福建物质结构研究所;吉林大学无机合成与制备国家重点实验室;
- 论文关键词：表面坑洞缺陷 ; 限域 ; 金属(氧化物)亚纳米簇 ; 稳定异相催化剂
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十七分会：纳米催化
- 语种：中文
- 分类号：TB383.1;O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十七分会 ; 纳米催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：152k
- 原文格式：D
- 会议级别：全国
摘要
金属(氧化物)亚纳米簇是工业催化中一类重要的催化剂~[1]。纳米簇暴露大量特殊活性位点而具有广阔应用前景,然而在催化过程中其容易偏析长大导致失活~[2]。我们报道了一种稳定纳米簇的策略,并通过温和的一锅水热法合成了CeO_2表面坑洞缺陷限域CuO纳米簇的杂化结构。透射电子显微镜表征显示氧化铈纳米颗粒表面密集分布小于5 nm的坑洞,CuO纳米簇限域在坑洞内。我们通过富氢环境下优先氧化CO测试所制备的复合结构催化剂,并与传统的CuO纳米颗粒负载CeO_2和Cu掺杂CeO_2催化剂作对比。研究表明这种结构的催化剂可以在120℃到200℃的宽温度窗口内近乎完全除去CO杂质,并且适合高温潮湿环境下长时间运行,而同组分的对照催化剂在同样条件下无法实现氢气流中完全氧化CO。这种合成策略有望扩展到其他材料体系,譬如CeO_2限域的Au,Pt纳米簇等催化剂。
Metal(oxide) cluster catalysts are critical in industry due to their efficient exposing of active sites.However,the catalyst would be inactive that caused by segregation and growth of metal clusters.We report a mild one-pot hydrothermal method to synthesize a catalyst with CuO clusters confining in pit-type defects of CeO_2.The performance of as-prepared catalyst was determined by preferential CO oxidation in H_2-rich streams(PROX),which is an important process in proton exchange membrane fuel cells.Compared with traditional CuO nanoparticles supported CeO_2 and Cu-doped CeO_2 samples,the confined catalyst exhibited nearly completely CO oxidation in the temperature range from 120 ℃ to 200 ℃,and showed long-time stability at high temperatures in humid PROX conditions.The strategy of confining metal(oxide) sub-nanoclusters in the pit-type defects of CeO_2 is expected to synthesize other systems,such as confined Pt,Au,to construct new types of synergistic catalysts.
Metal(oxide) cluster catalysts are critical in industry due to their efficient exposing of active sites.However,the catalyst would be inactive that caused by segregation and growth of metal clusters.We report a mild one-pot hydrothermal method to synthesize a catalyst with CuO clusters confining in pit-type defects of CeO_2.The performance of as-prepared catalyst was determined by preferential CO oxidation in H_2-rich streams(PROX),which is an important process in proton exchange membrane fuel cells.Compared with traditional CuO nanoparticles supported CeO_2 and Cu-doped CeO_2 samples,the confined catalyst exhibited nearly completely CO oxidation in the temperature range from 120 ℃ to 200 ℃,and showed long-time stability at high temperatures in humid PROX conditions.The strategy of confining metal(oxide) sub-nanoclusters in the pit-type defects of CeO_2 is expected to synthesize other systems,such as confined Pt,Au,to construct new types of synergistic catalysts.
引文
[1]Zhang,H.;Watanabe,T.;Okumura,M.;Haruta,M.;Toshima,N.Nat.Mater.2012,11,49-52.
[2]Delannoy,L.;Giorgio,S.;Mattei,J.G.;Henry,C.R.;El Kolli,N.;Méthivier,C.;Louis,C.Chem Cat Chem 2013,5,2707-2716.
[2]Delannoy,L.;Giorgio,S.;Mattei,J.G.;Henry,C.R.;El Kolli,N.;Méthivier,C.;Louis,C.Chem Cat Chem 2013,5,2707-2716.