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金属–有机框架中协同NH3捕获的配体插入机制
作者:小柯机器人 发布时间:2023/1/14 15:41:49

美国加州大学Long, Jeffrey R.团队报道了金属–有机框架中协同NH3捕获的配体插入机制。相关研究成果发表在2023年1月11日出版的国际知名学术期刊《自然》。

氨是农业和工业中的关键化学品,并通过哈伯-博世工艺大规模生产。该工艺使用甲烷作为燃料和氢气原料,对环境的影响促使人们需要更可持续的氨生产工艺。然而,许多使用可再生氢的策略与现有的氨分离方法不兼容。鉴于金属-有机框架(MOFs)的高表面积和结构和化学多功能性,它们有望用于氨分离,但大多数MOFs在暴露于这种腐蚀性气体时不可逆地结合氨或降解。

该文中,研究人员报道了一种可调的三维框架,该框架通过协同插入氨的金属-羧酸键可逆地结合氨,以形成致密的一维配位聚合物。这种不寻常的吸附机制提供了相当大的内在热管理,在高压和高温下,协同吸收氨会产生较大的工作能力。通过简单的合成改性,氨吸附的阈值压力可以进一步调整近五个数量级,这为开发高效氨吸附剂指明了更广泛的策略。

附:英文原文

Title: A ligand insertion mechanism for cooperative NH3 capture in metal–organic frameworks

Author: Snyder, Benjamin E. R., Turkiewicz, Ari B., Furukawa, Hiroyasu, Paley, Maria V., Velasquez, Ever O., Dods, Matthew N., Long, Jeffrey R.

Issue&Volume: 2023-01-11

Abstract: Ammonia is a critical chemical in agriculture and industry that is produced on a massive scale via the Haber–Bosch process1. The environmental impact of this process, which uses methane as a fuel and feedstock for hydrogen, has motivated the need for more sustainable ammonia production2,3,4,5. However, many strategies that use renewable hydrogen are not compatible with existing methods for ammonia separation6,7,8,9. Given their high surface areas and structural and chemical versatility, metal–organic frameworks (MOFs) hold promise for ammonia separations, but most MOFs bind ammonia irreversibly or degrade on exposure to this corrosive gas10,11. Here we report a tunable three-dimensional framework that reversibly binds ammonia by cooperative insertion into its metal–carboxylate bonds to form a dense, one-dimensional coordination polymer. This unusual adsorption mechanism provides considerable intrinsic thermal management12, and, at high pressures and temperatures, cooperative ammonia uptake gives rise to large working capacities. The threshold pressure for ammonia adsorption can further be tuned by almost five orders of magnitude through simple synthetic modifications, pointing to a broader strategy for the development of energy-efficient ammonia adsorbents.

DOI: 10.1038/s41586-022-05409-2

Source: https://www.nature.com/articles/s41586-022-05409-2

期刊信息
Nature:《自然》,创刊于1869年。隶属于施普林格·自然出版集团,最新IF:69.504
官方网址:http://www.nature.com/
 
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