Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, USA.
Nat Chem. 2012 Mar 18;4(5):383-8. doi: 10.1038/nchem.1295.
Green plants convert CO(2) to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO(2) 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 CO(2), 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 π-donor, and is rationalized by theoretical and experimental studies.
绿色植物通过光合作用将二氧化碳转化为糖来储存能量。我们报告了一种新型催化剂，它使用二氧化碳和氢气将能量储存在甲酸中。我们使用具有质子响应配体的均相铱催化剂，展示了第一个在温和条件下使用二氧化碳、甲酸盐和甲酸运行的可逆和可回收的储氢系统。该系统节能且环保，因为它在环境条件下运行，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。这种非凡的、可切换的催化活性归因于多功能配体，它起到质子传递体和强π-供体的作用，并通过理论和实验研究得到了合理化。
