Coupling electrocatalytic cathodic nitrate reduction with anodic formaldehyde oxidation at ultra-low potential over Cu2O

文献情報

出版日 2023-05-10

DOI 10.1039/D3EE00635B

インパクトファクター 38.532

著者

Lei Xiao, Weidong Dai, Shiyong Mou, Xiaoyan Wang, Qin Cheng

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要旨

Electrocatalytic ammonia (NH3) synthesis from nitrate (NO3−) is a promising alternative to the Haber–Bosch route that requires high energy input and carbon emissions. However, sluggish anodic oxygen evolution reaction (OER) kinetics requires a large overpotential (>1.23 V vs. RHE), severely restricting the electrocatalytic cathodic NO3− reduction reaction (NO3−RR). Herein, a HCHO oxidation reaction (FOR) was developed to achieve 300 mA cm−2 at 0.81 VRHE, which was 1.56 V lower than that of the OER (Pt). A superior HCOOH production rate of 9.64 mmol cm−2 h−1 was achieved over Cu2O, approaching the highest performance reported to date. Further investigation indicated that the anodic HCHO oxidation mechanism involves electrocatalytic oxidative dehydrogenation (EOD) and tandem reaction pathways. The tandem reaction features the electrocatalytic oxidation of cubic Cu2O to orthorhombic Cu(OH)2 and spontaneous reduction of Cu(OH)2 to Cu2O by HCHO. Subsequently, the two-electrode coupling FOR and NO3−RR wherein Cu2O is utilized at both anode and cathode requires an ultra-low cell voltage of −0.19 V to achieve 10 mA cm−2 and realizes the high faradaic efficiency of 99.77% for NO3− conversion to NH3. This strategy represents a novel transformative system for simultaneously treating pollutants (HCHO and NO3−) and yielding value-added chemicals (HCOOH and NH3).

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

Coupling electrocatalytic cathodic nitrate reduction with anodic formaldehyde oxidation at ultra-low potential over Cu2O

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