4.8 Article

Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures

Journal

NATURE CHEMISTRY
Volume 4, Issue 5, Pages 383-388

Publisher

NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1295

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Funding

  1. US Department of Energy and its Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences
  2. Japanese Ministry of Economy, Trade, and Industry
  3. CCHF [DE-SC0001298]
  4. US Department of Energy
  5. [DE-AC02-98CH10886]

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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.

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