Low-Valence Metal Single Atoms on Graphdiyne Promotes Electrochemical Nitrogen Reduction via M-to-N 2 π-Backdonation
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99 GENERAL AND MISCELLANEOUS↗
Engineering topics
Zou, Haiyuan
Publications and source records attributed to Zou, Haiyuan.
Few-Atom Copper Catalyst for the Electrochemical Reduction of CO to Acetate: Synergetic Catalysis between Neighboring Cu Atoms
Single-atom catalysts (SACs) are gaining increasing recognition because of their superior catalytic properties for various reactions. However, the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis. Herein, a synergetic interaction between neighboring Cu atoms of a few-atom catalyst (FAC) on graphdiyne is found to greatly enhance the production of acetate in CO electroreduction reaction relative to Cu SACs. In a 1.0 M KOH electrolyte, this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5 % and an ultrahigh relative purity of up to 97 wt% for liquid products, and excellent stability of over 23 h continuous electrolysis at -0.8 V versus reversible hydrogen electrode (RHE). Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH 2 CO* or the direct reaction of H 2 O with CH 2 CO*. Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective CO electroreduction toward acetate production.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction
Artificial nitrogen fixation through the nitrogen reduction reaction (NRR) under ambient conditions is a potentially promising alternative to the traditional energy-intensive Haber–Bosch process. For this purpose, efficient catalysts are urgently required to activate and reduce nitrogen into ammonia. Herein, by the combination of experiments and first-principles calculations, we demonstrate that copper single atoms, attached in a porous nitrogen-doped carbon network, provide highly efficient NRR electrocatalysis, which compares favorably with those previously reported. Benefiting from the high density of exposed active sites and the high level of porosity, the Cu SAC exhibits high NH 3 yield rate and Faradaic efficiency (FE), specifically ~53.3 μg$_{NH_3}$ h –1 mg cat –1 and 13.8% under 0.1 M KOH, ~49.3 μg$_{NH_3}$ h –1 mg cat –1 and 11.7% under 0.1 M HCl, making them truly pH-universal. They also show good stability with little current attenuation over 12 h of continuous operation. Cu–N 2 coordination is identified as the efficient active sites for the NRR catalysis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Direct Observation of Structural Evolution of Metal Chalcogenide in Electrocatalytic Water Oxidation
As one of the most remarkable oxygen evolution reaction (OER) electrocatalysts, metal chalcogenides have been intensively reported during the past few decades because of their high OER activities. It has been reported that electron-chemical conversion of metal chalcogenides into oxides/hydroxides would take place after the OER. However, the transition mechanism of such unstable structures, as well as the real active sites and catalytic activity during the OER for these electrocatalysts, has not been understood yet; therefore a direct observation for the electrocatalytic water oxidation process, especially at nano or even angstrom scale, is urgently needed. In this work, by employing advanced Cs-corrected transmission electron microscopy (TEM), a step by step oxidational evolution of amorphous electrocatalyst CoS x into crystallized CoOOH in the OER has been in situ captured: irreversible conversion of CoS x to crystallized CoOOH is initiated on the surface of the electrocatalysts with a morphology change via Co(OH) 2 intermediate during the OER measurement, where CoOOH is confirmed as the real active species. Besides, this transition process has also been confirmed by multiple applications of X-ray photoelectron spectroscopy (XPS), in situ Fourier-transform infrared spectroscopy (FTIR), and other ex situ technologies. Moreover, on the basis of this discovery, a high-efficiency electrocatalyst of a nitrogen-doped graphene foam (NGF) coated by CoS x has been explored through a thorough structure transformation of CoOOH. In conclusion, we believe this in situ and in-depth observation of structural evolution in the OER measurement can provide insights into the fundamental understanding of the mechanism for the OER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Progress towards quantum simulating the classical O ( 2 ) mode
We connect explicitly the classical $O(2)$ model in 1+1 dimensions, a model sharing important features with $U(1)$ lattice gauge theory, to physical models potentially implementable on optical lattices and evolving at physical time. Using the tensor renormalization group formulation, we take the time continuum limit and check that finite dimensional projections used in recent proposals for quantum simulators provide controllable approximations of the original model. We propose two-species Bose-Hubbard models corresponding to these finite dimensional projections at strong coupling and discuss their possible implementations on optical lattices using a $^{87}$Rb and $^{41}$K Bose-Bose mixture.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗