Frontiers, opportunities, and challenges in biochemical and chemical catalysis of CO2 fixation.
Frontiers, opportunities, and challenges in biochemical and chemical catalysis of CO2 fixation.
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DOI：
10.1021/cr300463y
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发表时间：
2013-08-14
期刊：
影响因子：
62.1
通讯作者：
Waldrop, Grover L.
中科院分区：
文献类型：
--
作者：
Appel, Aaron M.;Bercaw, John E.;Bocarsly, Andrew B.;Dobbek, Holger;DuBois, Daniel L.;Dupuis, Michel;Ferry, James G.;Fujita, Etsuko;Hille, Russ;Kenis, Paul J. A.;Kerfeld, Cheal A.;Morris, Robert H.;Peden, Charles H. F.;Portis, Archie R.;Ragsdale, Stephen W.;Rauchfuss, Thomas B.;Reek, Joost N. H.;Seefeldt, Lance C.;Thauer, Rudolf K.;Waldrop, Grover L.
未来50年，世界将面临两个与能源有关的主要问题。首先，全球范围内对逐渐耗尽的化石燃料储备（来自过去的光合作用）的竞争加剧将导致更高的成本，无论是在货币上还是政治上。第二，大气中的二氧化碳水平处于有记录以来的最高水平。预计进一步增加将对世界气候产生巨大和无法控制的影响。这些预计的影响超出了气候，延伸到海洋酸化，因为海洋是大气二氧化碳的主要汇。1.提供一个安全和二氧化碳中性的未来能源供应将需要转向非化石能源，如风能、太阳能、核能和地热能，并开发将这些新能源产生的能源转化为可以储存、运输和按需使用的形式的方法。二氧化碳是我们日常生活中使用的化石燃料的最终来源。这些化石燃料以气体、液体和固体的形式存在，我们可以从中选择最适合特定应用的形式。在可预见的未来，燃料选择的这种灵活性将是有益的。将碳固定到这些燃料中的过程是光合作用，即将阳光，水和二氧化碳生物转化为还原的有机物质。光合作用发生在非常大的规模。据估计，每年固定的二氧化碳净排放量为385× 109吨，2而总排放量则为2倍。二氧化碳固定的途径已经发展了数十亿年，并使用不同的机制和酶通过制造C-H和C-C键以及切割C-O键来处理二氧化碳。对CO2和CO还原的均相和非均相催化剂的研究也有助于我们理解合成燃料生产中涉及的C-C和C-H键形成反应以及C-O键裂解反应。因此，重大的科学和经济需要推动了二氧化碳作为燃料原料的发展。根据2008年贝尔/能源部的报告，4“阻碍将二氧化碳有效转化为含能产品的主要障碍是缺乏催化剂.”。这一背景说明了必须应对的挑战。由于这些考虑，在美国能源部基础能源科学司化学和生物化学理事会的主持下举办了一次关于二氧化碳化学的讲习班。该研讨会于2011年秋季举行，目的是评估催化和生物界对将二氧化碳直接转化为燃料问题的协同贡献，所有生物系统都必须从其环境中提取能量，以进行与生命本身相关的代谢过程。生物体已经进化到存在于各种各样的环境中，它们可以使用和相互转换来自各种来源的能量。除了六种已知的参与将CO2生物固定为有机碳的代谢途径之外，还有重要的
Two major energy-related problems confront the world in the next 50 years. First, increased worldwide competition for gradually depleting fossil fuel reserves (derived from past photosynthesis) will lead to higher costs, both monetarily and politically. Second, atmospheric CO2 levels are at their highest recorded level since records began. Further increases are predicted to produce large and uncontrollable impacts on the world climate. These projected impacts extend beyond climate to ocean acidification, because the ocean is a major sink for atmospheric CO2. 1 Providing a future energy supply that is secure and CO2-neutral will require switching to nonfossil energy sources such as wind, solar, nuclear, and geothermal energy and developing methods for transforming the energy produced by these new sources into forms that can be stored, transported, and used upon demand. Carbon dioxide is the ultimate source of the fossil fuels used in our daily lives. These fossil fuels exist as gases, liquids, and solids, from which we can select the form most suitable for a particular application. This flexibility in fuel choice will be beneficial for the foreseeable future. The process that drives carbon fixation into these fuels is photosynthesis, the biological conversion of sunlight, water, and carbon dioxide into reduced organic materials. Photosynthesis occurs on a very large scale. An estimated 385× 109 tons of carbon dioxide are fixed annually net, 2 and the gross value is larger by a factor of 2. 3 Pathways for CO2 fixation have evolved over billions of years and use diverse mechanisms and enzymes for processing CO2 by making C− H and C− C bonds and cleaving C− O bonds. Research on homogeneous and heterogeneous catalysts for CO2 and CO reduction has also contributed to our understanding of C− C and C− H bond formation reactions as well as C− O bond cleavage reactions involved in the production of synthetic fuels. Significant scientific and economic imperatives thus motivate the development of carbon dioxide as a feedstock for fuels. According to the 2008 Bell/DOE report, 4 “The major obstacle preventing efficient conversion of carbon dioxide into energy-bearing products is the lack of catalysts...” This background exemplifies the challenges that must be addressed. These considerations led to a workshop on CO2 chemistry carried out under the aegis of the Council on Chemical and Biochemical Sciences of the Basic Energy Sciences Division of the United States Department of Energy. Held in the fall of 2011, the workshop had the purpose of assessing synergistic contributions of the catalysis and biological communities to the problem of converting carbon dioxide directly into fuels.All biological systems must extract energy from their environments to carry out the metabolic processes associated with life itself. Living organisms have evolved to exist in an amazing variety of environments, and they can use and interconvert energy from a variety of sources. In addition to the six known metabolic pathways involved in the biological fixation of CO2 into organic carbon, there are also important
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