Journal ArticleDOI
Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction
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It is demonstrated that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N₂ to NH₃ at ambient temperature and pressure.Abstract:
The photocatalytic reduction of N₂ to NH₃ is typically hampered by poor binding of N₂ to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N₂ to NH₃ at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface.read more
Citations
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Construction of PdO–Pd interfaces assisted by laser irradiation for enhanced electrocatalytic N2 reduction reaction
Abstract: Due to the strong absorbability and excellent activating ability of palladium (Pd) element for N2, Pd-based materials have become one of the most promising catalysts for electrocatalytic N2 reduction reaction (NRR) applications, which is a low-cost and ecofriendly way for ammonia synthesis under ambient conditions. However, the lack of active sites and poor stability are still the major issues that restrain their catalytic activity. To solve these problems, PdO/Pd heterojunctions supported on carbon nanotubes (PdO/Pd/CNTs) with a controllable mass ratio of Pd to PdO were fabricated using ultraviolet laser irradiated PdO/CNTs in distilled water. Compared with PdO/CNTs, PdO/Pd/CNTs, especially the ten minutes irradiated one, present an optimal mass ratio of Pd (18%) to PdO (82%) and abundant PdO–Pd interfaces which can act as active sites for N2 dynamic activation and proton transitions, where the synergistic effect of Pd and PdO contributed to shorten the transmission route of protons and reduce the overpotential of the chemical reaction. Thus, the N2 conversion efficiency of PdO/Pd/CNTs was obviously improved, their faradaic efficiency reached up to 11.5% and NH3 yield was 18.2 μg mgcat.−1 h−1 at 0.1 V vs. RHE. Besides, this work will provide useful reference to design NRR catalysts with controllable surface states and defects by laser-assisted strategies.
Journal ArticleDOI
Local Modulation of Single-Atomic Mn Sites for Enhanced Ambient Ammonia Electrosynthesis
Lili Han,Lili Han,Machuan Hou,Pengfei Ou,Hao Cheng,Zhouhong Ren,Zhixiu Liang,J. Anibal Boscoboinik,Adrian Hunt,Iradwikanari Waluyo,Shusheng Zhang,Longchao Zhuo,Jun Song,Xijun Liu,Jun Luo,Huolin L. Xin +15 more
TL;DR: Rationally tuning the local structures of single-atomic active sites for the electrocatalytic N2 reduction reaction (NRR) remains an urgent but worthwhile research topic.
Journal ArticleDOI
Porous LaFeO3 nanofiber with oxygen vacancies as an efficient electrocatalyst for N2 conversion to NH3 under ambient conditions
Chengbo Li,Dongwei Ma,Shiyong Mou,Yongsong Luo,Benyuan Ma,Siyu Lu,Guanwei Cui,Quan Li,Qian Liu,Xuping Sun +9 more
TL;DR: In this article, a porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2.
Journal ArticleDOI
Spinel LiMn2O4 Nanofiber: An Efficient Electrocatalyst for N2 Reduction to NH3 under Ambient Conditions.
Chengbo Li,Jiali Yu,Li Yang,Jinxiu Zhao,Wenhan Kong,Ting Wang,Abdullah M. Asiri,Quan Li,Xuping Sun +8 more
TL;DR: A spinel LiMn2O4 nanofiber acts as a noble-metal-free electrocatalyst for NH3 synthesis with excellent performance under ambient conditions and possesses excellent electrochemical and structure stability.
Journal ArticleDOI
sp2/sp3 Framework from Diamond Nanocrystals: A Key Bridge of Carbonaceous Structure to Carbocatalysis
Xiaoguang Duan,Wenjie Tian,Huayang Zhang,Hongqi Sun,Zhimin Ao,Zongping Shao,Zongping Shao,Shaobin Wang,Shaobin Wang +8 more
TL;DR: Diamond nanocrystals in robust sp3 hybridization are appealing carbonaceous materials in the material community, whose structure can be transformed into unique sp2/sp3 nanohybrids as bulky nanodiam...
References
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Journal ArticleDOI
Electrochemical Photolysis of Water at a Semiconductor Electrode
Akira Fujishima,Kenichi Honda +1 more
TL;DR: Water photolysis is investigated by exploiting the fact that water is transparent to visible light and cannot be decomposed directly, but only by radiation with wavelengths shorter than 190 nm.
Journal ArticleDOI
The absolute electrode potential: an explanatory note (Recommendations 1986)
TL;DR: In this article, it is shown that in principle three reference levels can be chosen to measure an absolute value of the electrode potential, and a thermodynamic analysis of the components of the emf of an elec- trochemical cell is shown.
Journal ArticleDOI
Catalytic Reduction of Dinitrogen to Ammonia at a Single Molybdenum Center
TL;DR: In this paper, the authors explored the catalytic reduction of dinitrogen by molybdenum complexes that contain the [HIPTN3N]3- ligand.
Journal ArticleDOI
Quantum photoyield of diamond(111)—A stable negative-affinity emitter
TL;DR: In this paper, the secondary-electron energy distributions were analyzed for an unreconstructed diamond (111) surface (type-$\mathrm{II}b), gem-quality blue-white semiconductor).
Proceedings ArticleDOI
The HITRAN molecular spectroscopic database and HAWKS (HITRAN atmospheric workstation)
Laurence S. Rothman,Curtis P. Rinsland,Aaron Goldman,Steven T. Massie,David P. Edwards,Jean-Marie Flaud,Agnes Perrin,Claude Camy-Peyret,V. Dana,Y.-Y. Mandin,J. Schroeder,Robert R. Gamache,R. B. Wattson,Kouichi Yoshino,Kelly Chance,Kenneth W. Jucks,Linda R. Brown,V. Nemtchinov,Prasad Varanasi +18 more
TL;DR: The data and features that have been added or replaced since the previous edition of HITRAN are described and instances of critical data that are forthcoming are cited.