Journal ArticleDOI
Au Sub-Nanoclusters on TiO2 toward Highly Efficient and Selective Electrocatalyst for N2 Conversion to NH3 at Ambient Conditions.
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TLDR
It is demonstrated that by using Au sub-nanoclusters embedded on TiO2 (Au loading is 1.542 wt%), the electrocatalytic N2 reduction reaction (NRR) is indeed possible at ambient condition and with very high and stable production yield.Abstract:
As the NN bond in N2 is one of the strongest bonds in chemistry, the fixation of N2 to ammonia is a kinetically complex and energetically challenging reaction and, up to now, its synthesis is still heavily relying on energy and capital intensive Haber-Bosch process (150-350 atm, 350-550 °C), wherein the input of H2 and energy are largely derived from fossil fuels and thus result in large amount of CO2 emission. In this paper, it is demonstrated that by using Au sub-nanoclusters (≈0.5 nm ) embedded on TiO2 (Au loading is 1.542 wt%), the electrocatalytic N2 reduction reaction (NRR) is indeed possible at ambient condition. Unexpectedly, NRR with very high and stable production yield (NH3 : 21.4 µg h-1 mg-1cat. , Faradaic efficiency: 8.11%) and good selectivity is achieved at -0.2 V versus RHE, which is much higher than that of the best results for N2 fixation under ambient conditions, and even comparable to the yield and activation energy under high temperatures and/or pressures. As isolated precious metal active centers dispersed onto oxide supports provide a well-defined system, the special structure of atomic Au cluster would promote other important reactions besides NRR for water splitting, fuel cells, and other electrochemical devices.read more
Citations
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Journal ArticleDOI
Catalysts for nitrogen reduction to ammonia
Shelby L. Foster,Sergio I. Perez Bakovic,Royce D. Duda,Sharad Maheshwari,Ross D. Milton,Shelley D. Minteer,Michael J. Janik,Julie N. Renner,Lauren F. Greenlee +8 more
TL;DR: A review of the state of the art and scientific needs for heterogeneous electrocatalysts for electrochemical reduction of dinitrogen to ammonia can be found in this article, with a particular focus on how mechanistic understanding informs catalyst design.
Journal ArticleDOI
A Review of Electrocatalytic Reduction of Dinitrogen to Ammonia under Ambient Conditions
TL;DR: In this paper, the authors summarized the recent progress on the electrochemical nitrogen reduction reaction (NRR) at ambient temperature and pressure from both theoretical and experimental aspects, aiming at extracting instructive perceptions for future NRR research activities.
Journal ArticleDOI
A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements
Suzanne Zamany Andersen,Viktor Colic,Sungeun Yang,Sungeun Yang,Jay A. Schwalbe,Adam C. Nielander,Joshua M. McEnaney,Kasper Enemark-Rasmussen,Jon G. Baker,Aayush R. Singh,Brian A. Rohr,Michael J. Statt,Sarah J. Blair,Stefano Mezzavilla,Jakob Kibsgaard,Peter Christian Kjærgaard Vesborg,Matteo Cargnello,Stacey F. Bent,Thomas F. Jaramillo,Ifan E. L. Stephens,Jens K. Nørskov,Ib Chorkendorff +21 more
TL;DR: A protocol for the electrochemical reduction of nitrogen to ammonia enables isotope-sensitive quantification of the ammonia produced and the identification and removal of contaminants, and should help to prevent false positives from appearing in the literature.
Journal ArticleDOI
Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat.-1 h-1 for N2 Electrochemical Reduction over Ru Single-Atom Catalysts.
Zhigang Geng,Yan Liu,Xiangdong Kong,Pai Li,Kan Li,Zhongyu Liu,Junjie Du,Miao Shu,Rui Si,Jie Zeng +9 more
TL;DR: This work not only develops a superior electrocatalyst for NH3 production, but also provides a guideline for the rational design of highly active and robust single-atom catalysts.
Journal ArticleDOI
Boron-Doped Graphene for Electrocatalytic N2 Reduction
Xiaomin Yu,Peng Han,Zengxi Wei,Linsong Huang,Zhengxiang Gu,Sijia Peng,Jianmin Ma,Gengfeng Zheng +7 more
TL;DR: In this paper, a boron-doped graphene was used as an efficient metal-free N2 reduction electrocatalyst, achieving a NH3 production rate of 9.8μg·hr−1·cm−2 and one of the highest reported faradic efficiencies of 10.8% at −0.5 V versus reversible hydrogen electrode in aqueous solutions at ambient conditions.
References
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Journal ArticleDOI
Challenges in reduction of dinitrogen by proton and electron transfer
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Journal ArticleDOI
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TL;DR: The rate of ammonia synthesis over a nanoparticle ruthenium catalyst can be calculated directly on the basis of a quantum chemical treatment of the problem using density functional theory, and offers hope for computer-based methods in the search for catalysts.
Journal ArticleDOI
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