Near-unity electrochemical conversion of nitrate to ammonia on crystalline nickel porphyrin-based covalent organic frameworks

文献情報

出版日 2022-11-23

DOI 10.1039/D2EE02647C

インパクトファクター 38.532

著者

Mingzi Sun

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要旨

Electrochemical nitrate reduction, which has attracted rapidly increasing attention over recent years, can potentially enable the indirect fixation of atmospheric N2 as well as the efficient removal of nitrate from industrial wastewater. It is, however, limited by the lack of efficient and low-cost electrocatalysts available so far. To address this challenge, we here demonstrate a two-dimensional nickel porphyrin-based covalent organic framework (COF) as a potential candidate for the first time. The product has a highly ordered molecular structure with abundant square-shaped nanopores. In neutral solution, the reduction of nitrate ions at different concentrations from ammonia is realized with a great selectivity of ∼90% under a mild overpotential, a remarkable production rate of up to 2.5 mg h−1 cm−2, a turnover frequency of up to 3.5 s−1, and an intrinsic stability that is best delivered under pulse electrolysis. This cathodic reaction can also be coupled with the oxygen evolution reaction to enable full-cell electrolysis at high efficiency. Theoretical computations indicate that nickel centers can stably adsorb nitrate, and facilitate its subsequent reduction by lowering the energy barrier of the rate-determining step.

掲載誌

Energy & Environmental Science

CiteScore: 32.34

自己引用率: 3.4%

年間論文数: 481

Energy & Environmental Science is an international journal dedicated to publishing exceptionally important and high quality, agenda-setting research tackling the key global and societal challenges of ensuring the provision of energy and protecting our environment for the future. The scope is intentionally broad and the journal recognises the complexity of issues and challenges relating to energy conversion and storage, alternative fuel technologies and environmental science. For work to be published it must be linked to the energy-environment nexus and be of significant general interest to our community-spanning readership. All scales of studies and analysis, from impactful fundamental advances, to interdisciplinary research across the (bio)chemical, (bio/geo)physical sciences and chemical engineering disciplines are welcomed. Topics include, but are not limited to, the following: Solar energy conversion and photovoltaics Solar fuels and artificial photosynthesis Fuel cells Hydrogen storage and (bio) hydrogen production Materials for energy systems Capture, storage and fate of CO2, including chemicals and fuels from CO2 Catalysis for a variety of feedstocks (for example, oil, gas, coal, biomass and synthesis gas) Biofuels and biorefineries Materials in extreme environments Environmental impacts of energy technologies Global atmospheric chemistry and climate change as related to energy systems Water-energy nexus Energy systems and networks Globally applicable principles of energy policy and techno-economics

Near-unity electrochemical conversion of nitrate to ammonia on crystalline nickel porphyrin-based covalent organic frameworks

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