Underpotential Deposition of Copper Clusters on Sulfur and Nitrogen Co‐Doped Graphite Foam for the Oxygen Reduction Reaction

Xu, Jingsong; Li, Rui; Zeng, Rongguang; Li, Yingru; Pan, Qifa; Zhong, Hang; Chen, Jun

doi:10.1002/celc.201901546

Cited by 5 publications

(3 citation statements)

References 56 publications

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“…S13). Obvious negative shifts for the low-valence S species are observed for these samples, which is due to the electron transfer from Cu to S dopants [42,48]. Remarkably, the Cu-S peak for Cu NPs/SrGO appears at the lowest energy, indicating the strongest metal-support interaction.…”

Section: Preparation and Characterization Of Srgo-supported Cu Sas Cu...mentioning

confidence: 85%

电化学溶出法尺寸可控合成铜基氧还原反应催化剂: 从纳米粒子到原子团簇和单原子

Zhao

et al. 2022

Sci. China Mater.

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Size-controllable synthesis of non-noble metal particles ranging from nanometer to subnanometer and atomic level is of great significance for demonstrating the size effects of metallic catalysts towards oxygen reduction reaction (ORR) catalysis. Herein, we propose an electrochemical leaching strategy for the top-down synthesis of Cu nanoparticles (NPs), atomic clusters (ACs) and single atoms (SAs) on sulfur-doped reduced graphene oxide (SrGO). Within this strategy, Cu NPs (about 8 nm) were electrodeposited and subsequently controllably downsized to ACs (about 2 nm) and SAs (<1 nm) via a stripping voltammetry method by adjusting the termination potential. The effective control in the size of active Cu species allowed us to conveniently investigate the size effect of Cu on ORR in multiscale. Single-atom Cu exhibited good ORR performance with a half-wave potential of 0.86 V and an electron transfer number of 3.98, as well as a long-term stability, much superior to other larger Cu particles. Our findings open a new avenue for top-down synthesis of metal particles with desirable sizes, which will effectively benefit the future design of size-controlled ORR electrocatalysts.

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Section: Preparation and Characterization Of Srgo-supported Cu Sas Cu...mentioning

confidence: 85%

电化学溶出法尺寸可控合成铜基氧还原反应催化剂: 从纳米粒子到原子团簇和单原子

Zhao

et al. 2022

Sci. China Mater.

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“…The X-ray diffraction (XRD) spectra further elucidate that Cu is dispersed in the form of single atom, where the (002) plane peak of BAPB-MoS 2 within 2 h intercalation time shifts to the higher angle compared with pristine MoS 2 (Figure 3d). This can be explained by the formation of Cu-S bonds, [25,26] which decreases interlayer spacing. On the contrary, when the intercalation time was extended to 12 h and overmuch Cu atoms were inserted into the layers, Cu atoms would aggregate and stretch the interlayer spacing (Figure 3d).…”

Section: Atomic Structure Of Mos 2 With An Interlayer Biatomic Pair B...mentioning

confidence: 99%

Interlayer Biatomic Pair Bridging the van der Waals Gap for 100% Activation of 2D Layered Material

Wang,

Yang,

Ding

et al. 2024

Advanced Materials

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Two‐dimensional (2D) layered materials are regarded as prospective catalyst candidates due to their advantageous atomic exposure ratio. Nevertheless, the predominant population of atoms residing on the basal plane, exhibiting saturated coordination, exhibit inert behavior, while a mere fraction of atoms located at the periphery display reactivity. Here, we report a novel approach to attain complete atom activation in 2D layered materials through the construction of an interlayer bi‐atomic pair bridge. The atoms in question have been strategically optimized to achieve a highly favorable state for the adsorption of intermediates. This optimization results in the introduction of new gap states around the Fermi level. Moreover, the presence of the interlayer bridge facilitates the electron transfer across the van der Waals gap, thereby enhancing the reaction kinetics. The hydrogen evolution reaction exhibits an impressive ultrahigh current density of 2000 mA cm–2 at 397 mV, surpassing the pristine MoS2 by approximately two orders of magnitude (26 mA cm–2 at 397 mV). Our study provides new insights for enhancing the efficacy of 2D layered catalysts.This article is protected by copyright. All rights reserved

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“…Transition metal (TM) clusters with precise atomic numbers can offer multiple active sites, tune the size-dependent catalytic activity [26], and allow them to find the highest reactivity for the activation and dissociation of strong chemical bonds from CO 2 . Xu et al [27] reported a facile underpotential deposition technique to fabricate Cu clusters on carbonaceous substrates via rationally introducing S dopants in graphite foam. The obtained free-standing electrode exhibited high activity and excellent long-term stability toward oxygen reduction reaction.…”

Section: Introductionmentioning

confidence: 99%

DFT Study on the CO2 Reduction to C2 Chemicals Catalyzed by Fe and Co Clusters Supported on N-Doped Carbon

Xue

Yang

et al. 2022

Nanomaterials

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The catalytic conversion of CO2 to C2 products through the CO2 reduction reaction (CO2RR) offers the possibility of preparing carbon-based fuels and valuable chemicals in a sustainable way. Herein, various Fen and Co5 clusters are designed to screen out the good catalysts with reasonable stability, as well as high activity and selectivity for either C2H4 or CH3CH2OH generation through density functional theory (DFT) calculations. The binding energy and cohesive energy calculations show that both Fe5 and Co5 clusters can adsorb stably on the N-doped carbon (NC) with one metal atom anchored at the center of the defected hole via a classical MN4 structure. The proposed reaction pathway demonstrates that the Fe5-NC cluster has better activity than Co5-NC, since the carbon–carbon coupling reaction is the potential determining step (PDS), and the free energy change is 0.22 eV lower in the Fe5-NC cluster than that in Co5-NC. However, Co5-NC shows a better selectivity towards C2H4 since the hydrogenation of CH2CHO to CH3CHO becomes the PDS, and the free energy change is 1.08 eV, which is 0.07 eV higher than that in the C-C coupling step. The larger discrepancy of d band center and density of states (DOS) between the topmost Fe and sub-layer Fe may account for the lower free energy change in the C-C coupling reaction. Our theoretical insights propose an explicit indication for designing new catalysts based on the transition metal (TM) clusters supported on N-doped carbon for multi-hydrocarbon synthesis through systematically analyzing the stability of the metal clusters, the electronic structure of the critical intermediates and the energy profiles during the CO2RR.

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Underpotential Deposition of Copper Clusters on Sulfur and Nitrogen Co‐Doped Graphite Foam for the Oxygen Reduction Reaction

Cited by 5 publications

References 56 publications

电化学溶出法尺寸可控合成铜基氧还原反应催化剂: 从纳米粒子到原子团簇和单原子

电化学溶出法尺寸可控合成铜基氧还原反应催化剂: 从纳米粒子到原子团簇和单原子

Interlayer Biatomic Pair Bridging the van der Waals Gap for 100% Activation of 2D Layered Material

DFT Study on the CO2 Reduction to C2 Chemicals Catalyzed by Fe and Co Clusters Supported on N-Doped Carbon

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