Journal ArticleDOI
Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid.
Katherine A. Brown,Derek F. Harris,Molly B. Wilker,Andrew J. Rasmussen,Nimesh Khadka,Hayden Hamby,Stephen Keable,Gordana Dukovic,John W. Peters,Lance C. Seefeldt,Paul W. King +10 more
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TLDR
It is shown that cadmium sulfide (CdS) nanocrystals can be used to photosensitize the nitrogenase molybdenum-iron (MoFe) protein, where light harvesting replaces ATP hydrolysis to drive the enzymatic reduction of N2 into NH3.Abstract:
The splitting of dinitrogen (N2) and reduction to ammonia (NH3) is a kinetically complex and energetically challenging multistep reaction. In the Haber-Bosch process, N2 reduction is accomplished at high temperature and pressure, whereas N2 fixation by the enzyme nitrogenase occurs under ambient conditions using chemical energy from adenosine 5'-triphosphate (ATP) hydrolysis. We show that cadmium sulfide (CdS) nanocrystals can be used to photosensitize the nitrogenase molybdenum-iron (MoFe) protein, where light harvesting replaces ATP hydrolysis to drive the enzymatic reduction of N2 into NH3 The turnover rate was 75 per minute, 63% of the ATP-coupled reaction rate for the nitrogenase complex under optimal conditions. Inhibitors of nitrogenase (i.e., acetylene, carbon monoxide, and dihydrogen) suppressed N2 reduction. The CdS:MoFe protein biohybrids provide a photochemical model for achieving light-driven N2 reduction to NH3.read more
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Emerging Two-Dimensional Nanomaterials for Electrocatalysis
Huanyu Jin,Chunxian Guo,Xin Liu,Jinlong Liu,Anthony Vasileff,Yan Jiao,Yao Zheng,Shi-Zhang Qiao +7 more
TL;DR: The fundamental relationships between electronic structure, adsorption energy, and apparent activity for a wide variety of 2D electrocatalysts are described with the goal of providing a better understanding of these emerging nanomaterials at the atomic level.
Journal ArticleDOI
Beyond fossil fuel-driven nitrogen transformations.
Jingguang G. Chen,Jingguang G. Chen,Richard M. Crooks,Lance C. Seefeldt,Kara L. Bren,R. Morris Bullock,Marcetta Y. Darensbourg,Patrick L. Holland,Brian M. Hoffman,Michael J. Janik,Anne K. Jones,Mercouri G. Kanatzidis,Paul W. King,Kyle M. Lancaster,Sergei V. Lymar,Peter H. Pfromm,William F. Schneider,Richard R. Schrock +17 more
TL;DR: Research prospects for more sustainable routes to nitrogen commodity chemicals are reviewed, considering developments in enzymatic, homogeneous, and heterogeneous catalysis, as well as electrochemical, photochemical, and plasma-based approaches.
Journal ArticleDOI
Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions
TL;DR: In this article, the rational design of electrocatalysts and photo(electro) catalysts for N2 reduction to NH3 under ambient conditions is highlighted, with a special emphasis on the relationship between their physicochemical properties and NH3 production performance.
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
Au Sub-Nanoclusters on TiO2 toward Highly Efficient and Selective Electrocatalyst for N2 Conversion to NH3 at Ambient Conditions.
TL;DR: 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.
References
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Semiconductor Clusters, Nanocrystals, and Quantum Dots
TL;DR: In this article, the authors focus on the properties of quantum dots and their ability to join the dots into complex assemblies creates many opportunities for scientific discovery, such as the ability of joining the dots to complex assemblies.
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Experimental Determination of the Extinction Coefficient of CdTe, CdSe, and CdS Nanocrystals
TL;DR: In this article, the extinction coefficient per mole of nanocrystals at the first exitonic absorption peak, e.g., for high-quality CdTe, CdSe, and CdS, was found to be strongly dependent on the size of the nanocrystal, between a square and a cubic dependence.
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Electronic wave functions in semiconductor clusters: experiment and theory
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Mechanism of Nitrogen Fixation by Nitrogenase: The Next Stage
TL;DR: This paper presents a meta-analyses of the chiral stationary phase replacement of Na6(CO3)(SO4)2, Na2SO4, and Na2CO3 of the H2O/O2 mixture and shows clear patterns in the response of these two types of molecules to each other in a stationary phase.
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Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach
Luigi Carbone,Concetta Nobile,Milena De Giorgi,Fabio Della Sala,Giovanni Morello,Pierpaolo Pompa,Martin Hÿtch,Etienne Snoeck,Angela Fiore,Isabella R. Franchini,Monica Nadasan,Albert F Silvestre,Letizia Chiodo,Stefan Kudera,Roberto Cingolani,Roman Krahne,Liberato Manna +16 more
TL;DR: A seeded-growth approach is reported to the synthesis of asymmetric core-shell CdSe/CdS nanorods with regular shapes and narrow distributions of rod diameters and lengths, the latter being easily tunable up to 150 nm.