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Activation of Small Inert Molecules

小惰性分子的活化

基本信息

批准号：
04241104
负责人：
HIDAI Masanobu
金额：
$ 85.7万
依托单位：
University of Tokyo
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research on Priority Areas
财政年份：
1992
资助国家：
日本
起止时间：
1992 至 1994
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-04241104/
关键词：
small inert molecule dinitrogen methane carbon dioxide metal cluster solid surface

项目摘要

The Objective of this research project lines in the establishment of chemical transformaitons using small inert molecules such as dinitrogen and methane which are abundant on earth, and carbon dioxide, the increase of which in the atmosphere arises from the use of fossil fuel by the human being and is becoming a serious environmental problems on a global scale. This is the fundamental and basic research towards the development of ideal chemical processes using carbon dioxide and methane as the simple carbon resourse and dinitrogen as the simple nitrogen resource to synthesize valuable organic compounds.Efficient activation and chemical utilization of these small inert molecules are one of the most challenging subjects in chemistry. The main achievements in this project are described below.1) The coordinated dinitrogen in molybdenum and tungsten phosphine complexes has been converted into nitrogen-heterocyclic compounds such as pyrrole and aminopyrrole via a series of reactions under mi … More ld conditions. Indole derivatives have also been synthesized from dinitrogen by using titanium systems. These results will open a new chemistry of nitrogen fixation where a variety of organo-nitrogen compounds are directly prepared from molecular nitrogen.2) Electrochemical reduction of carbon dioxide on a copper electrode gives rise to the formation of methane, ethane, and ethanol. The reaction has been revealed to proceed through the formaiton of carbon monoxide as an intermediate on the electrode.3) Selective electrochemical reduction of carbon dioxide to methanol has been for the first time realized by using redox enzymes as electrocatalysts.4) Photoelectrochemical reduction of carbon dioxide on the p-type silicon electrode modified with ultrafine copper particles has led to the formation of methane and ethylene at a more positive potential than on a copper metal electrode.5) New reactions have been developed which transform methane and carbon monoxide into acetic acids by using copper catalyst. This provides the first example of the carbon-carbon bond formation reactions of methane under mild conditions. Less

本研究项目的目的是利用地球上丰富的小惰性分子如二氮和甲烷以及二氧化碳建立化学转化，人类使用化石燃料导致大气中二氧化碳的增加，并正在成为全球范围内严重的环境问题。这是以二氧化碳和甲烷为简单碳源，以二氮为简单氮源合成有机化合物的基础性研究，有效活化和化学利用这些惰性小分子是化学领域最具挑战性的课题之一。本课题的主要研究成果如下：1）在室温下，通过一系列反应，将钼、钨膦配合物中的配位二氮转化为吡咯、氨基吡咯等氮杂环化合物 ...更多信息 LD条件。吲哚衍生物也已经通过使用钛系统由二氮合成。这些结果将开辟一种新的固氮化学，其中各种有机氮化合物直接从分子氮制备。2）二氧化碳在铜电极上的电化学还原引起甲烷、乙烷和乙醇的形成。3）首次实现了以氧化还原酶为电催化剂的二氧化碳选择性电化学还原为甲醇的反应; 4）在p-ZnO电极上实现了二氧化碳的光电化学还原; 5）在p-ZnO电极上实现了二氧化碳的电化学还原，并在p-ZnO电极上实现了二氧化碳的电化学还原用超细铜颗粒修饰的型硅电极导致甲烷和乙烯在比铜金属电极更正的电势下形成。已经开发了使用铜催化剂将甲烷和一氧化碳转化为乙酸的新反应。这提供了甲烷在温和条件下的碳-碳键形成反应的第一个实例。少