Realizing Negatively Charged Metal Atoms through Controllable d‐Electron Transfer in Ternary Ir1−xRhxSb Intermetallic Alloy for Hydrogen Evolution Reaction (Adv. Energy Mater. 25/2022)

Lin, Zhiping; Xiao, Beibei; Huang, Min; Yan, Linghui; Wang, Zongpeng; Huang, Yucong; Shen, Shijie; Zhang, Qinghua; Gu, Lin; Zhong, Wen‐De

doi:10.1002/aenm.202270108

Cited by 13 publications

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“…[ 1,2 ] Electrochemical hydrogen evolution reaction (HER) can utilize clean energy efficiently, such as wind and solar energy, to produce high‐purity H 2 in an acidic medium. [ 3–5 ] Currently, Pt is the most widely used catalyst in HER, but its high cost and the disadvantage of being prone to be poisoned during the catalytic processes restrict the further improvement of catalyst performance. [ 6,7 ] Therefore, developing electrocatalysts that have high catalytic activity, excellent electrical conductivity, and remarkable stability is crucial for energy science.…”

Section: Introductionmentioning

confidence: 99%

Single Cobalt Atoms Immobilized on Palladium‐Based Nanosheets as 2D Single‐Atom Alloy for Efficient Hydrogen Evolution Reaction

Yang

et al. 2023

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Single‐atom alloys (SAAs) display excellent electrocatalytic performance by overcoming the scaling relationships in alloys. However, due to the lack of a unique structure engineering design, it is difficult to obtain SAAs with a high specific surface area to expose more active sites. Herein, single Co atoms are immobilized on Pd metallene (Pdm) support to obtain Co/Pdm through the design of the engineered morphology of Pd, realizing the preparation of ultra‐thin 2D SAA. The unsaturated coordination environments combined with the unique geometric and electronic structures realize the modulation of the d‐band center and the redistribution of charges, generating highly active electronic states on the surface of Co/Pdm. Benefiting from the synergistic interaction and spillover effect, the Co/Pdm electrocatalyst exhibits outstanding hydrogen evolution reaction (HER) performance in both acid and alkaline solutions, especially with a Tafel slope of 8.2 mV dec−1 and a low overpotential of 24.7 mV at 10 mA cm−2 in the acidic medium, which outperforms commercial Pt/C and Pd/C. This work highlights the successful preparation of 2D ultra‐thin SAA, which provides a new strategy for the preparation of HER electrocatalyst with high efficiency, activity, and stability.

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Section: Introductionmentioning

confidence: 99%

Single Cobalt Atoms Immobilized on Palladium‐Based Nanosheets as 2D Single‐Atom Alloy for Efficient Hydrogen Evolution Reaction

Yang

et al. 2023

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“…[ 1–3 ] Such a four‐electron transfer reaction involving multiple reaction intermediates exhibits sluggish OER kinetics, leading to substantial overpotentials and losses in energy efficiency. [ 4–7 ] To date, noble metal oxides (such as IrO 2 or RuO 2 ) afford the most satisfactory activity among various OER electrocatalysts. [ 8–10 ] In particular, improved intrinsic OER activities of Ir‐based catalysts have been proposed by various strategies including alloying, [ 11–13 ] formation of hybrids with other metal oxides, [ 14 ] amorphous or low‐crystalline characteristics, [ 15 ] and participation of lattice oxygen.…”

Section: Introductionmentioning

confidence: 99%

Rhenium Suppresses Iridium (IV) Oxide Crystallization and Enables Efficient, Stable Electrochemical Water Oxidation

Huo

Zhou

Jin

et al. 2023

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IrO2 as benchmark electrocatalyst for acidic oxygen evolution reaction (OER) suffers from its low activity and poor stability. Modulating the coordination environment of IrO2 by chemical doping is a methodology to suppress Ir dissolution and tailor adsorption behavior of active oxygen intermediates on interfacial Ir sites. Herein, the Re‐doped IrO2 with low crystallinity is rationally designed as highly active and robust electrocatalysts for acidic OER. Theoretical calculations suggest that the similar ionic sizes of Ir and Re impart large spontaneous substitution energy and successfully incorporate Re into the IrO2 lattice. Re‐doped IrO2 exhibits a much larger migration energy from IrO2 surface (0.96 eV) than other dopants (Ni, Cu, and Zn), indicating strong confinement of Re within the IrO2 lattice for suppressing Ir dissolution. The optimal catalysts (Re: 10 at%) exhibit a low overpotential of 255 mV at 10 mA cm−2 and a high stability of 170 h for acidic OER. The comprehensive mechanism investigations demonstrate that the unique structural arrangement of the Ir active sites with Re‐dopant imparts high performance of catalysts by minimizing Ir dissolution, facilitating *OH adsorption and *OOH deprotonation, and lowering kinetic barrier during OER. This study provides a methodology for designing highly‐performed catalysts for energy conversion.

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“…This reveals an electron transfer from Co to Rh or Ir and their strong electronic interactions, similar to those between Co and Ru in the RuCo‐CAT NRAs. [ 37 ]…”

Section: Resultsmentioning

confidence: 99%

Creating Dual Active Sites in Conductive Metal‐Organic Frameworks for Efficient Water Splitting

Yan

Zhang

et al. 2023

Advanced Energy Materials

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the ever-increasing energy demand and the environmental problems associated with the use of fossil fuels. Due to its high energy density and environmental friendliness, hydrogen fuel is the cleanest energy carrier. [1] Among the industrial hydrogen generation techniques, [2] electrochemical water electrolysis is a simple process, and no other by-products are produced, which fulfills the concept of clean technology. However, the sluggish kinetics of the two half-reactions, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), limit the energy conversion efficiency. [3] To date, the precious metal Pt and Ru/Ir oxides are the most active electrocatalysts for HER and OER, respectively. However, the high price and limited reserves hinder their application on large scale. To further improve the efficiency of water splitting, high-performance and less expensive bifunctional electrocatalysts for HER and OER are required, and recent research includes the use of transitionmetal oxides, sulfides, nitrides, carbides, and borides. [4,5] However, their overall activities for water splitting were still much lower than those of the coupled Pt/C and IrO 2 /RuO 2 commercial catalysts. Thus, it is imperative to develop bifunctional electrocatalysts with HER and OER activities, which simultaneously outperform Pt/C and IrO 2 /RuO 2 .Metal-organic frameworks (MOFs) are typically porous crystalline polymers that are composed of metallic nodes and organic linkers. MOFs possess abundantly periodic porosity, tunable functionality, and versatile framework topologies, leading to their potential applications in the fields of energy storage and conversion, gas sorption and separation, sensors, biomedicine, and proton/ion conductors. [6][7][8][9][10][11] In particular, conductive MOFs have attracted considerable attention for catalyzing various chemical reactions, including OER, HER, oxygen reduction reaction, and CO 2 reduction, due to their improved reaction dynamics. [12][13][14][15][16][17][18][19] To overcome the drawbacks of bulk conductive MOFs such as the exposure limitations of their surface areas and metallic nodes to electrolytes, several strategies have been recently explored including reducing the size of MOFs to several nanometers or even atomic level, [20,21] defect engineering, [22] creating cavities inside MOFs, [23] introducing different metallic nodes into MOFs, [24,25] and anchoring MOFs on conductive substrates. [26] Through these strategies, the catalytic activities of the conductive MOFs were significantly enhanced especially for HER and OER compared to theirThe achievement of bifunctional metal-organic frameworks (MOFs) remains a huge challenge due to their lack of dual active sites. Herein, dual sites in the Co-catecholate (Co-CAT) are created through Ru, Ir, or Rh doping for overall water splitting. Among them, RuCo-CAT exhibits excellent bifunctional activities, outperforming benchmarked Pt/C for the hydrogen evolution reaction (HER) and RuO 2 for the oxygen evolution reaction (OER). The theoretical ...

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Realizing Negatively Charged Metal Atoms through Controllable d‐Electron Transfer in Ternary Ir₁₋_xRh_xSb Intermetallic Alloy for Hydrogen Evolution Reaction (Adv. Energy Mater. 25/2022)

Cited by 13 publications

References 0 publications

Single Cobalt Atoms Immobilized on Palladium‐Based Nanosheets as 2D Single‐Atom Alloy for Efficient Hydrogen Evolution Reaction

Single Cobalt Atoms Immobilized on Palladium‐Based Nanosheets as 2D Single‐Atom Alloy for Efficient Hydrogen Evolution Reaction

Rhenium Suppresses Iridium (IV) Oxide Crystallization and Enables Efficient, Stable Electrochemical Water Oxidation

Creating Dual Active Sites in Conductive Metal‐Organic Frameworks for Efficient Water Splitting

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