氧化铜-氧化亚铜界面催化的碳-碳键氧化裂解研究
详细信息 查看官网全文
- 英文论文题名：Cu_2O-Cu_2O interface catalyzed C-C bond oxidative cleavage
- 论文作者：王敏 ; 吕建民 ; 王峰
- 英文论文作者：Min Wang ; Jianmin Lu ; Feng Wang ; National Laboratory for Clean Energy ; State Key Laboratory of Catalysis ; Dalian Institute of Chemical Physics ; Chinese Academy of Sciences
- 年：2016
- 作者机构：中国科学院大连化学物理研究所催化国家重点实验室清洁能源国家实验室;
- 论文关键词：界面 ; 氧化亚铜 ; C-C键氧化裂解 ; 氧化 ; 催化
- 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-第十五分会：表界面结构调控与催化
- 语种：中文
- 分类号：O621.251
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十五分会 ; 表界面结构调控与催化
- 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：220k
- 原文格式：D
- 会议级别：全国
摘要
相界面活性位的认识,以及与催化性能关系的认知是多相催化研究的一个重要问题。虽然模型催化剂已有研究,但是对于真实的催化剂体系,由于其复杂性,研究甚少。氧化亚铜是一个应用广泛的催化材料[1]。我们通过部分氧化的方法制备了氧化亚铜/氧化铜异相界面结构[2]。通过高倍电子显微镜技观测到大约5 nm的Cu O纳米嵌入在Cu_2O表层。Cu_2O表层没有完全被氧化成Cu O,可以充分暴漏Cu O-Cu_2O异相界面结构。这样一种可被底物分子所接触的异相界面结构在催化中有广泛的应用前景。在三丁胺氧化反应中,传统催化反应过程和生物体内酶催化过程,键能C-N优先被裂解。而Cu O-Cu_2O异相界面催化剂高选择性的断裂键能更大的C-C键,生成甲酰产物。为甲酰胺的制备提供了一种新的方法。
Unveiling the local structure of active site in interfacial phase,and establishing a close relationship with catalytic activity have remained central issues for heterogeneous catalysis.Despite of numerous studies have been pursued in model catalysts,the examples on real catalyst are still limited.We show how to control the surface oxidation of pristine Cu_2O and enable it a highly active and selective catalyst in oxidation reaction.We discover that the partial oxidation generates an embedded structure in the topmost surface layers of Cu_2O.It is very encouraging that such embedded Cu O-Cu_2O structure shows very high activity towards C–C bond cleavage and excellent selectivity towards formamides in trialkylamines oxidation.
Unveiling the local structure of active site in interfacial phase,and establishing a close relationship with catalytic activity have remained central issues for heterogeneous catalysis.Despite of numerous studies have been pursued in model catalysts,the examples on real catalyst are still limited.We show how to control the surface oxidation of pristine Cu_2O and enable it a highly active and selective catalyst in oxidation reaction.We discover that the partial oxidation generates an embedded structure in the topmost surface layers of Cu_2O.It is very encouraging that such embedded Cu O-Cu_2O structure shows very high activity towards C–C bond cleavage and excellent selectivity towards formamides in trialkylamines oxidation.
引文
[1]Wang,M.;Lu,J.;Ma,J.;Zhang,Z.;Wang,F.;Angew.Chem.Int.Ed.,2015,54(47):14061.
[2]Wang,M.;Gu,X.;Su,H.;Lu,J.;Ma,J.;Yu,M.;Zhang,Z.;Wang.F.;J.Catal.,2015,330:458.
[2]Wang,M.;Gu,X.;Su,H.;Lu,J.;Ma,J.;Yu,M.;Zhang,Z.;Wang.F.;J.Catal.,2015,330:458.