Dynamic coordination transformation of active sites in single-atom MoS<sub>2</sub> catalysts for boosted oxygen evolution catalysis

Ran, Nian; Song, Erhong; Wang, Youwei; Zhou, Yao; Li, Jianjun

doi:10.1039/d1ee02750f

Cited by 49 publications

(38 citation statements)

References 98 publications

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“…In addition, some new characterization and analytical tools at the atomic and molecular scale, such as high-resolution scanning electrochemical cell microscopy and electron backscatter diffraction [106], can be developed for the accurate structure clarification. (3) Very recent report indicated that the dynamic transformations of coordination environment and composition of CO 2 RR catalyst have been verified by operando XAFS characterization [107,108]. The monitoring of real-time structural information of dual-atomic active sites under dynamic CO 2 RR operating conditions should be further exploited by single or multiple in-situ or operando techniques to unveil the underlying reconstruction or deactivation of dual-atomic active sites [109][110][111][112].…”

Section: Conclusion and Perspectivementioning

confidence: 99%

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Qiu

Wang

et al. 2022

Sci. China Mater.

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The electrochemical CO 2 reduction reaction (CO 2 RR) to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality. Constant endeavors have been devoted to the exploration of high-efficiency catalyst with rapid reaction kinetics, low energy input, and high selectivity. In addition to the maximum metal atomic utilization and unique catalytic performance of single-atom catalyst (SAC), dual-atomic-site catalysts (DASCs) offer more sophisticated and tunable atomic structure through the modulations of another adjacent metal atom, which can bring new opportunities for CO 2 RR as a deeper extension of SACs and have recently aroused surging interest. In this review, we highlight the recent advances on DASCs for enhancing CO 2 RR. First, the classification, synthesis, and identification of DASCs are provided according to the geometric structure and electronic configuration of dual-atomic active sites. Then, the catalytic applications of DASCs in CO 2 RR are categorized based on marriage-type, hetero-nuclear, and homo-nuclear dual-atomic sites. Particularly, the structure-activity relationship of DASCs in CO 2 RR is elaborately summarized through systematically analyzing the reaction pathways and the atom structures. Finally, the opportunities and challenges are proposed for inspiring the design of future DASCs with high structural accuracy and high CO 2 RR activity and selectivity.

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Section: Conclusion and Perspectivementioning

confidence: 99%

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Qiu

Wang

et al. 2022

Sci. China Mater.

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“…It is well known that metals and their oxides and hydroxides mostly play a vital role in OER. [27][28][29] Among many metal materials, Co-based materials are probed to be suitable for efficient OER electrocatalysts. [30][31][32] This is a profit from the electronic structure of Co.…”

Section: Introductionmentioning

confidence: 99%

Ion‐change promoting Co nanoparticles@N‐doped carbon framework on Co₂SiO₄/rGO support forming “double‐triple‐biscuit” structure boosts oxygen evolution reaction

Pei

Yang

Dong

et al. 2023

Carbon Neutralization

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Exploring economic and high-performance electrocatalysts to decrease the overpotential of oxygen evolution reaction (OER) and facilitate its reaction kinetics is a frontier subject in line with green energy. Herein, metal-organic framework (MOF)-derived Co nanoparticles@N-doped carbon (Co NPs@N,C) is rationally designed on sandwich-like cobalt silicate/reduced graphene oxide (Co 2 SiO 4 /rGO) support to acquire Co NPs@N,C/Co 2 SiO 4 /rGO "double-triplebiscuit"-like structure as enhanced OER electrocatalysts. Co NPs@N,C on Co 2 SiO 4 /rGO support optimizes its geometric architecture and introduces new active sites. The "double-triple-biscuit"-like Co NPs@N,C/Co 2 SiO 4 /rGO structure achieves excellent OER ability compared with the existing materials based on transition metal silicates (TMSs). The overpotential of 278 mV is achieved at the current density of 10 mA cm −2 , and it is prominently higher than Co 2 SiO 4 /rGO support (390 mV). This excellent OER activity is rooted in its structural peculiarity, enabling efficient ion and electron transport. Co NPs@N,C are highly dispersed on the Co 2 SiO 4 /rGO support, increasing the active sites and avoiding self-aggregation of Co NPs in the OER process. This work combines the advantages of Co 2 SiO 4 /rGO support with the triple biscuits' structure and MOF to implement the preparation of boosted Co NPs@N,C/Co 2 SiO 4 /rGO, and it opens a new avenue for designing novel architectures to promote the OER activity of TMSs.

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“…Huang and co-workers demonstrated that different coordination structures of Cu single atoms in C 3 N 4 -supported Cu catalysts led to different reaction pathways in CO 2 hydrogenation . Liu and co-workers reported that high catalytic activity for the oxygen evolution reaction was achieved by a coordination transformation of TMO x in atomically dispersed TMO x @MoS 2 (TM = Mn, Fe, and Co) . Similarly, tuning the coordination environment of Ag single atoms in CN-supported Ag catalysts from AgN 4 to AgN 2 C 2 reduced the transfer barrier for photogenerated electrons to Ag sites, thus improving the photocatalytic performance …”

Section: Introductionmentioning

confidence: 99%

Tailoring the Electronic Structure of Single Ag Atoms in Ag/WO₃ for Efficient NO Reduction by CO in the Presence of O₂

Chen

Liu

et al. 2023

ACS Catal.

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Developing efficient catalysts for the selective catalytic reduction of NO x by CO (CO-SCR) is the key challenge for commercializing this technology. Ag-based catalysts with relatively low costs are promising but widely believed to be not efficient enough for this reaction. Here, we demonstrate that atomically dispersed Ag supported on ordered mesoporous WO 3 (m-WO 3 ) can serve as a highly active catalyst for CO-SCR under O 2 -containing conditions. By altering the amount of the Ag precursor, the local environment of the Ag atom coordinated with the O atom can be tailored. Furthermore, at 250 °C and an O 2 /CO ratio of 2.5:1, 0.3Ag/m-WO 3 (0.3 wt % Ag) with six-coordinated Ag−O exhibited much better catalytic performance than 5 Ag/m-WO 3 (5 wt % Ag) with twocoordinated Ag−O (e.g., 0.43 vs 0.02 mol NO g Ag −1 h −1 in the reaction rate) and previously reported Ag-based catalysts in the literature. The theoretical calculations confirm that the six-coordinated Ag atoms in 0.3Ag/m-WO 3 possess a more positive oxidation state and a higher d-band center than the two-coordinated Ag atoms in 5Ag/m-WO 3 , promoting its bonding strength with coadsorption of the critical intermediates of N 2 O* and CO*. This work provides a feasible route for regulating the local environment of a Ag single atomic catalyst to enhance its catalytic property for CO-SCR.

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Dynamic coordination transformation of active sites in single-atom MoS₂ catalysts for boosted oxygen evolution catalysis

Abstract: The development of low-cost and efficient electrocatalysts for the oxygen evolution reaction (OER) is critical for enhancing the efficiency of water-splitting reaction. Although MoS2 is a promising hydrogen evolution electrocatalyst,...

Cited by 49 publications

References 98 publications

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Ion‐change promoting Co nanoparticles@N‐doped carbon framework on Co₂SiO₄/rGO support forming “double‐triple‐biscuit” structure boosts oxygen evolution reaction

Tailoring the Electronic Structure of Single Ag Atoms in Ag/WO₃ for Efficient NO Reduction by CO in the Presence of O₂

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Dynamic coordination transformation of active sites in single-atom MoS2 catalysts for boosted oxygen evolution catalysis

Abstract: The development of low-cost and efficient electrocatalysts for the oxygen evolution reaction (OER) is critical for enhancing the efficiency of water-splitting reaction. Although MoS2 is a promising hydrogen evolution electrocatalyst,...

Cited by 49 publications

References 98 publications

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Ion‐change promoting Co nanoparticles@N‐doped carbon framework on Co2SiO4/rGO support forming “double‐triple‐biscuit” structure boosts oxygen evolution reaction

Tailoring the Electronic Structure of Single Ag Atoms in Ag/WO3 for Efficient NO Reduction by CO in the Presence of O2

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Dynamic coordination transformation of active sites in single-atom MoS₂ catalysts for boosted oxygen evolution catalysis

Ion‐change promoting Co nanoparticles@N‐doped carbon framework on Co₂SiO₄/rGO support forming “double‐triple‐biscuit” structure boosts oxygen evolution reaction

Tailoring the Electronic Structure of Single Ag Atoms in Ag/WO₃ for Efficient NO Reduction by CO in the Presence of O₂