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作 者:张德善 梁永鹏 杨钰 佟振合[1,2] 吴骊珠 De-Shan Zhang;Yong-Peng Liang;Yu Yang;Chen-Ho Tung;Li-Zhu Wu(Key Laboratory of Photochemical Conversion and Optoelectronic Materials,New Cornerstone Science Laboratory,Technical Institute of Physics and Chemistry,Chinese Academy of Sciences,Beijing 100190,China;School of Future Technology,University of Chinese Academy of Sciences,Beijing 100049,China)
机构地区:[1]中国科学院理化技术研究所,光化学转换与功能材料重点实验室,新基石科学实验室,北京100190 [2]中国科学院大学未来技术学院,北京100049
出 处:《科学通报》2025年第7期835-849,共15页Chinese Science Bulletin
基 金:国家重点研发计划(2022YFA1502900,2022YFA1503200,2021YFA1500100);国家自然科学基金(22193013,21933007,22088102);中国科学院战略重点研究项目(XDB17000000);新基石科学基金资助。
摘 要:氨(NH_(3))作为化肥的重要成分和潜在的清洁能源载体,其可持续生产对于应对全球能源需求和环境问题意义重大.传统的Haber-Bosch工艺在高温和高压条件下,将氮气(N_(2))和氢气(H_(2))催化转化成NH_(3).该工艺支撑了全球近半数人口的粮食生产,但其存在的高能耗、高排放等问题无法满足可持续发展的要求.生物固氮酶能够在温和条件下实现N_(2)到NH_(3)的高效转化,为绿色高效驱动N_(2)还原提供了重要的参考.在过去几十年中,研究人员受天然酶活性中心的组成和结构特性的启发,模拟制备了一系列新型均相分子催化剂和多相催化剂,以实现高效人工固氮.本文综述了近年来人工光合固氮领域的重要进展,详细分析了N_(2)还原过程中的热力学和动力学挑战及其催化机理,并对人工光合固氮领域所面临的挑战与未来发展方向进行了讨论.With the continuous growth of global energy demand and the increasingly severe environmental challenges,the development of clean and sustainable alternative energy sources has become a key priority for countries worldwide.Ammonia(NH_(3)),as one of the most important basic chemical raw materials and a potential clean energy carrier,plays a crucial role in supporting agricultural production and industrial development.Nitrogen(N_(2)),one of the most abundant inert molecules in the atmosphere,requires a substantial amount of energy and efficient catalysts to be reduced to NH_(3).Since the early 20th century,the Haber-Bosch process has dominated industrial NH_(3)production,where iron-based catalysts synthesize NH_(3)from N_(2)and H_(2)under high temperature(350-450℃)and high pressure(150-200 atm).However,this process is highly energy-intensive,consuming about 2%of the world’s total energy supply and contributing to over 1%of global carbon emissions.These significant energy and environmental costs raise concerns about the sustainability of the Haber-Bosch process.Despite efforts to develop new coal chemical and H_(2)production technologies to improve energy efficiency and reduce carbon emissions,the issues of high energy consumption and pollution remain largely unresolved.As a result,there has been increasing interest in exploring alternative methods for N_(2)reduction that are mild,efficient,and sustainable.This has greatly stimulated research focused on achieving efficient N_(2)reduction to synthesize NH_(3)under mild conditions.The high-efficiency N_(2)fixation achieved by nitrogenases under ambient conditions has inspired researchers to study the structure and electronic properties of these enzymes to design efficient and stable artificial N_(2)fixation catalysts.Natural nitrogenases are capable of reducing N_(2)to NH_(3)under mild conditions with high efficiency and selectivity,offering valuable insights for the development of artificial systems.In recent years,significant progress has been made in the field o
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