EAGER: SusChEM: Carbon-Carbon Bond Formation Driven By the Water-Gas Shift Reaction

化学催化的一些主要目标是降低实现重要化学转化所需的能量输入，减少产生所需最终产物所需的材料（溶剂、试剂等）的数量。在这个由化学部化学催化项目资助的项目中，Scott E. Denmark教授正在进行研究，以改进与工业相关的化学过程，即水煤气转移反应（WGSR）。该反应在各种基本化学反应中用于形成碳-碳键。本研究项目的目标是用污染较少的试剂取代产生大量废物的含金属试剂。WGSR被大规模用于为大批量化学过程生产氢气。该反应通常是通过将一氧化碳和水在固体催化剂上结合产生氢气和二氧化碳来完成的。这项研究旨在用更少的副产品和溶剂形成新的碳-碳键。丹麦教授的学生确定了最有效的催化剂，使所需的化学反应在温和的反应条件下。该项目旨在减少精细化工生产中的浪费。2005年，美国国家研究委员会（National Research Council）发布了一份具有里程碑意义的报告《化学工业的可持续性》（Sustainability in Chemical Industry），确定了八大“重大挑战”，其中第一个是“绿色和可持续化学与工程”。该报告呼吁进行研究，以“确定适当的溶剂，控制热条件，净化，回收和配制防止浪费的产品，这些产品对环境无害，经济上可行，并总体上支持更好的社会生活质量”。尽管所有的研究都是为了提高WGSR的效率，但该工艺仅用于使用多相催化产生氢气。然而，除了氢甲酰化之外，没有其他碳-碳键形成反应被开发出来，利用WGSR的还原潜力。该项目确定了重要的碳-碳键形成反应，这些反应需要化学计量量的还原剂，并在合适的催化剂或催化剂组合存在的情况下，用水和一氧化碳的混合物取代还原剂。这项研究是培养新科学家创造性思维的良好平台。

Some of the major objectives of chemical catalysis are to lower the energy input required to effect important chemical transformations and reduce the amount of materials needed (solvents, reagents, etc.) to generate the desired end product. In this project funded by the Chemical Catalysis Program of the Chemistry Division, Professor Scott E. Denmark is conducting research to improve an industrially relevant chemical process, the Water Gas Shift Reaction (WGSR). The reaction is used to form of carbon-carbon bonds in a variety of fundamental chemical reactions. The goal of this research project is to replace metal-containing reagents that generate large amounts of waste products with less polluting reagents. The WGSR is used on an enormous scale to generate hydrogen for high volume chemical processes. The reaction is generally done by combining carbon monoxide and water over a solid catalyst to produce hydrogen and carbon dioxide. The research seeks to form new carbon-carbon bonds with fewer by-products and solvents. Professor Denmark's students identify the most efficient catalysts to enable the desired chemical reaction under mild reaction conditions. The project is designed to reduce waste in fine chemical manufacturing.The landmark report "Sustainability in the Chemical Industry" published by the National Research Council in 2005, identified eight "Grand Challenges" the first of which is "Green and Sustainable Chemistry and Engineering". The report called for research to "Identify appropriate solvents, control thermal conditions, and purify, recover, and formulate products that prevent waste and that are environmentally benign, economically viable, and generally support a better societal quality of life". Despite all of the research into improving the efficiency of the WGSR, the process is exclusively used for generation of hydrogen using heterogeneous catalysis. However, outside of hydroformylation, no other carbon-carbon bond forming reactions have been developed that harness the reducing potential of the WGSR. This project identifies important carbon-carbon bond forming reactions that require stoichiometric amounts of a reducing agent and replaces that agent with the combination of water and carbon monoxide in the presence of a suitable catalyst or catalyst combination. This research is an good platform for training new scientists to think creatively.