Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures
Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures
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DOI：
10.1038/nchem.1295
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发表时间：
2012-05-01
期刊：
影响因子：
21.8
通讯作者：
Fujita, Etsuko
中科院分区：
文献类型：
--
作者：
Hull, Jonathan F.;Himeda, Yuichiro;Fujita, Etsuko
绿色植物通过光合作用将二氧化碳转化为糖以储存能量。我们报告了一种新型催化剂，它使用二氧化碳和氢气在甲酸中储存能量。使用具有质子响应配体的均相铱催化剂，我们展示了第一个可逆且可回收的储氢系统，该系统使用二氧化碳、甲酸盐和甲酸在温和条件下运行。该系统节能且绿色，因为它在接近环境条件下运行，使用水作为溶剂，产生高压无二氧化碳氢气，并使用 pH 值来控制氢气的产生或消耗。非凡且可切换的催化活性归因于多功能配体，它充当质子中继和强π供体，并通过理论和实验研究合理化。
Green plants convert CO2 to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO2 and hydrogen to store energy in formic acid. Using a homogeneous iridium catalyst with a proton-responsive ligand, we show the first reversible and recyclable hydrogen storage system that operates under mild conditions using CO2, formate and formic acid. This system is energy-efficient and green because it operates near ambient conditions, uses water as a solvent, produces high-pressure CO-free hydrogen, and uses pH to control hydrogen production or consumption. The extraordinary and switchable catalytic activity is attributed to the multifunctional ligand, which acts as a proton-relay and strong pi-donor, and is rationalized by theoretical and experimental studies.