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Open accessJournal ArticleDOI: 10.1038/S41467-021-21750-Y

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

04 Mar 2021-Nature Communications (Springer Science and Business Media LLC)-Vol. 12, Iss: 1, pp 1449-1449
Abstract: Direct experimental observations of the interface structure can provide vital insights into heterogeneous catalysis. Examples of interface design based on single atom and surface science are, however, extremely rare. Here, we report Cu–Sn single-atom surface alloys, where isolated Sn sites with high surface densities (up to 8%) are anchored on the Cu host, for efficient electrocatalytic CO2 reduction. The unique geometric and electronic structure of the Cu–Sn surface alloys (Cu97Sn3 and Cu99Sn1) enables distinct catalytic selectivity from pure Cu100 and Cu70Sn30 bulk alloy. The Cu97Sn3 catalyst achieves a CO Faradaic efficiency of 98% at a tiny overpotential of 30 mV in an alkaline flow cell, where a high CO current density of 100 mA cm−2 is obtained at an overpotential of 340 mV. Density functional theory simulation reveals that it is not only the elemental composition that dictates the electrocatalytic reactivity of Cu–Sn alloys; the local coordination environment of atomically dispersed, isolated Cu–Sn bonding plays the most critical role. The understanding of catalytic reactions at the atomic interface is vital; however, the characterization and mechanism studies of atomically dispersed catalysts remain challenging. Here, the authors demonstrate Cu–Sn surface alloys with isolated Sn atoms on a Cu host to achieve efficient CO2 to CO conversion.

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Topics: Overpotential (55%), Electrocatalyst (51%)

8 results found

Open accessDOI: 10.1016/J.APMATE.2021.10.003
Yufei Jia1, Fei Li1, Ke Fan1, Licheng Sun2  +2 moreInstitutions (3)
15 Nov 2021-
Abstract: The extensive consumption of fossil fuels has caused the rapid increase in the CO2 level in the atmosphere, forcing people to find a clean and efficient technology of CO2 conversion to alleviate CO2 emissions and develop value-added products. Among various CO2 conversion systems, electroreduction of CO2 to value-added chemicals is a feasible way for practical applications. Copper, the only metal that can catalyze CO2 reduction to multi-carbon products, has attracted the most attention among various catalysts. However, slow reaction kinetics, low product selectivity, as well as poor stability are the main drawbacks of single metallic Cu-based catalysts. Such issues can be addressed by introducing second metal in Cu-based catalysts. Here, we summarize the recent progress relating to the Cu-based bimetallic electrocatalysts for CO2 reduction, and discuss the composition and structure effects on the activity and selectivity of electrochemical CO2 reduction. Last, we outline the challenges and perspectives on electrocatalysts for this field. We expect that this review can provide new insights into the further development of Cu-based bimetallic electrocatalysts for CO2 reduction.

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3 Citations

Open accessJournal ArticleDOI: 10.1016/J.RSER.2021.111922
Zhangsen Chen1, Gaixia Zhang1, Hangrong Chen2, Jai Prakash3  +2 moreInstitutions (4)
Abstract: Electrochemical CO2 reduction reaction (ECO2RR) offers an opportunity to sustainably convert CO2 into value-added fuels and chemicals by using the electricity that could be generated by renewable energies. Recently, enormous efforts are focused on the development of metal-based catalysts for the selective ECO2RR with high efficiency. Multi-metallic catalyst design emerges as one of the most promising strategies for the promotion of the Faradaic efficiency (FE), the current density, and the lowering of the overpotential of the catalysts for ECO2RR. The synergistic effects of the different metal sites in the hybrid catalysts are of significance for the enhancement of the ECO2RR performance. This review summarizes the rational design of multi-metallic catalysts, including alloy, atomically dispersed multi-metallic sites, and others, along with the popular metal elements studied in multi-metallic catalysts to clarify the advantages of different metal elements for ECO2RR. The density functional theory (DFT) simulations and advanced in-situ characterizations that contribute to demystifying the synergies between metal elements are highlighted. Challenges and outlook concerning the catalyst design and reaction mechanism of multi-metallic catalysts for ECO2RR are also discussed.

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Open accessJournal ArticleDOI: 10.3390/MOLECULES26216501
He He1, Hudson Haocheng Wang, Junjian Liu1, Xujun Liu2  +2 moreInstitutions (2)
28 Oct 2021-Molecules
Abstract: Due to excellent performance properties such as strong activity and high selectivity, single-atom catalysts have been widely used in various catalytic reactions. Exploring the application of single-atom catalysts and elucidating their reaction mechanism has become a hot area of research. This article first introduces the structure and characteristics of single-atom catalysts, and then reviews recent preparation methods, characterization techniques, and applications of single-atom catalysts, including their application potential in electrochemistry and photocatalytic reactions. Finally, application prospects and future development directions of single-atom catalysts are outlined.

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Journal ArticleDOI: 10.1002/CCTC.202100966
Xiang Tan1, Xiang Tan2, Hu Li2, Song Yang2Institutions (2)
13 Sep 2021-Chemcatchem
Abstract: Single‐atom catalysts (SACs) have attracted extensive attention since their emergence. During the single‐atomic catalytic process, the “active center” exists in the form of atomical monodispersion, with nearly 100 % utilization of metal atoms. Uniform and atomically dispersed catalytic centers give SACs pronounced reaction activity and chemical selectivity. Here, we review the development processes, synthetic strategies, characterization methods, and applications of SACs in CO2 reductive upgrading. Also, a comparison of SACs with conventional heterogeneous catalysts in catalytic CO2 reduction is made and discussed. SACs have built a bridge between homogeneous and heterogeneous catalysis and have the advantages of both, showing a broad prospect in the field of catalysis.

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Topics: Atom (order theory) (55%)

Journal ArticleDOI: 10.1021/ACSAMI.1C09128
Abstract: Tuning bimetallic effects is a promising strategy to guide catalytic properties. However, the nature of these effects can be difficult to assess and compare due to the convolution with other factors such as the catalyst surface structure and morphology and differences in testing environments. Here, we investigate the impact of atomic-scale bimetallic effects on the electrochemical CO2 reduction performance of Cu-based catalysts by leveraging a systematic approach that unifies protocols for materials synthesis and testing and enables accurate comparisons of intrinsic catalytic activity and selectivity. We used the same physical vapor deposition method to epitaxially grow Cu(100) films decorated with a small amount of noble or base metal atoms and a combination of experimental characterization and first-principles calculations to evaluate their physicochemical and catalytic properties. The results indicate that the metal atoms segregate to under-coordinated Cu sites during physical vapor deposition, suppressing CO reduction to oxygenates and hydrocarbons and promoting competing pathways to CO, formate, and hydrogen. Leveraging these insights, we rationalize bimetallic design principles to improve catalytic selectivity for CO2 reduction to CO, formate, oxygenates, or hydrocarbons. Our study provides one of the most extensive studies on Cu bimetallics for CO2 reduction, establishing a systematic approach that is broadly applicable to research in catalyst discovery.

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Topics: Bimetallic strip (51%)


49 results found

Journal ArticleDOI: 10.1021/JP047349J
Abstract: We present a method for calculating the stability of reaction intermediates of electrochemical processes on the basis of electronic structure calculations. We used that method in combination with detailed density functional calculations to develop a detailed description of the free-energy landscape of the electrochemical oxygen reduction reaction over Pt(111) as a function of applied bias. This allowed us to identify the origin of the overpotential found for this reaction. Adsorbed oxygen and hydroxyl are found to be very stable intermediates at potentials close to equilibrium, and the calculated rate constant for the activated proton/electron transfer to adsorbed oxygen or hydroxyl can account quantitatively for the observed kinetics. On the basis of a database of calculated oxygen and hydroxyl adsorption energies, the trends in the oxygen reduction rate for a large number of different transition and noble metals can be accounted for. Alternative reaction mechanisms involving proton/electron transfer to ...

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Topics: Overpotential (59%), Reaction rate constant (57%), Oxygen (53%) ... show more

5,473 Citations

Open accessJournal ArticleDOI: 10.1038/S41467-018-07882-8
Maksim Kunitski1, Nicolas Eicke2, Pia Huber1, Jonas Köhler1  +12 moreInstitutions (2)
Abstract: Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.

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Topics: Ionization (55%), Neon (54%)

4,138 Citations

Open accessJournal ArticleDOI: 10.1063/1.4812323
18 Jul 2013-APL Materials
Abstract: Accelerating the discovery of advanced materials is essential for human welfare and sustainable, clean energy. In this paper, we introduce the Materials Project (, a core program of the Materials Genome Initiative that uses high-throughput computing to uncover the properties of all known inorganic materials. This open dataset can be accessed through multiple channels for both interactive exploration and data mining. The Materials Project also seeks to create open-source platforms for developing robust, sophisticated materials analyses. Future efforts will enable users to perform ‘‘rapid-prototyping’’ of new materials in silico, and provide researchers with new avenues for cost-effective, data-driven materials design. © 2013 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.

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Topics: Materials informatics (59%)

4,076 Citations

Journal ArticleDOI: 10.1039/C0EE00071J
Abstract: Density functional theory calculations explain copper's unique ability to convert CO2 into hydrocarbons, which may open up (photo-)electrochemical routes to fuels.

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Topics: Metal carbon dioxide complex (67%), Hydrocarbon (56%), Copper (53%) ... show more

1,691 Citations

Journal ArticleDOI: 10.1002/ANIE.200504386
28 Apr 2006-Angewandte Chemie
Abstract: The fuel cell is a promising alternative to environmentally unfriendly devices that are currently powered by fossil fuels. In the polymer electrolyte membrane fuel cell (PEMFC),the main fuel is hydrogen,which through its reaction with oxygen produces electricity with water as the only by-product. To make PEMFCs economically viable,there are several problems that should be solved; the main one is to find more effective catalysts than Pt for the oxygen reduction reaction (ORR),1/2 O 2 + 2H + + 2e = H2O. The design of inexpensive,stable,and catalytically active materials for the ORR will require fundamental breakthroughs,and to this end it is important to develop a fundamental understanding of the catalytic process on different materials. Herein,we describe how variations in the electronic structure determine trends in the catalytic activity of the ORR across the periodic table. We show that Pt alloys involving 3d metals are better catalysts than Pt because the electronic structure of the Pt atoms in the surface of these alloys has been modified slightly. With this understanding,we hope that electrocatalysts can begin to be designed on the basis of fundamental insight.

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1,593 Citations