Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Sun, Yunfei; Xue, Ziqian; Liu, Qinglin; Jia, Yongzhong; Li, Yinle; Liu, Kang; Lin, Yiyang; Liu, Min; Su, Cheng‐Yong

doi:10.1038/s41467-021-21595-5

Cited by 409 publications

(297 citation statements)

References 78 publications

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“…In [88], with permission from the American Chemical Society [91,92], MOF [93], Graphdiyne [94], MXene [95,96], and nitrogen-doped carbon [97].…”

Section: D Ru-based Catalystmentioning

confidence: 99%

“…SACs may be the best solution for Ru-based catalysts because of the maximum utilization of Ru atoms and the exposure of active centers. Presently, Ru SACs with different loadings have been prepared on various carriers, such as phosphors [ 91 , 92 ], MOF [ 93 ], Graphdiyne [ 94 ], MXene [ 95 , 96 ], and nitrogen-doped carbon [ 97 ].…”

Section: Maximum Utilization: Single-atom Ru-based Catalysismentioning

confidence: 99%

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Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

et al. 2021

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The investigation of highly effective, durable, and cost-effective electrocatalysts for the hydrogen evolution reaction (HER) is a prerequisite for the upcoming hydrogen energy society. To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy, electrochemical water-splitting is considered the most promising, environmentally friendly, and efficient way to produce pure hydrogen. Compared with the commonly used platinum (Pt)-based catalysts, ruthenium (Ru) is expected to be a good alternative because of its similar hydrogen bonding energy, lower water decomposition barrier, and considerably lower price. Analyzing and revealing the HER mechanisms, as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable. In this review, the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced. Moreover, four major strategies to improve the performance of Ru-based electrocatalysts, including electronic effect modulation, support engineering, structure design, and maximum utilization (single atom) are discussed. Finally, the challenges, solutions and prospects are highlighted to prompt the practical applications of Ru-based electrocatalysts for HER.

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“…In [88], with permission from the American Chemical Society [91,92], MOF [93], Graphdiyne [94], MXene [95,96], and nitrogen-doped carbon [97].…”

Section: D Ru-based Catalystmentioning

confidence: 99%

Section: Maximum Utilization: Single-atom Ru-based Catalysismentioning

confidence: 99%

Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

et al. 2021

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“…[28] More importantly, MOFs feature high capability for cleaving the H-OH bond, and they can act as the co-catalysts to couple with other electrocatalysts for boosting the HER kinetics in alkaline or neutral media. [29][30][31] Despite so many advantages, fine-tuning the interfacial electron interaction between metal NPs and MOF supports for HER is so far rarely reported. Therefore, it is expected that the reciprocal decoration effect between NPs and functionalized MOF sheets can be favorable in pH-universal hydrogen evolution.…”

Section: Introductionmentioning

confidence: 99%

Electronic Modulation Caused by Interfacial Ni‐O‐M (M=Ru, Ir, Pd) Bonding for Accelerating Hydrogen Evolution Kinetics

Deng

et al. 2021

Angewandte Chemie

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Designing definite metal‐support interfacial bond is an effective strategy for optimizing the intrinsic activity of noble metals, but rather challenging. Herein, a series of quantum‐sized metal nanoparticles (NPs) anchored on nickel metal–organic framework nanohybrids (M@Ni‐MOF, M=Ru, Ir, Pd) are rationally developed through a spontaneous redox strategy. The metal‐oxygen bonds between the NPs and Ni‐MOF guarantee structural stability and sufficient exposure of the surface active sites. More importantly, such precise interfacial feature can effectively modulate the electronic structure of hybrids through the charge transfer of the formed Ni‐O‐M bridge and then improves the reaction kinetics. As a result, the representative Ru@Ni‐MOF exhibits excellent hydrogen evolution reaction (HER) activity at all pH values, even superior to commercial Pt/C and recent noble‐metal catalysts. Theoretical calculations deepen the mechanism understanding of the superior HER performance of Ru@Ni‐MOF through the optimized adsorption free energies of water and hydrogen due to the interfacial‐bond‐induced electron redistribution.

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“…Recently, the atomically dispersed Ru was introduced on the metal-organic framework (MOF) Ni-1,4-benzenedicarboxylic (BDC) to regulate the electronic structure of Ni for improved HER performance. [5] Furthermore, employing microenvironment engineering to immobilize single Pt atoms in MXene nanosheets (Mo 2 TiC 2 T x ) and onion-like carbon nanospheres supports could greatly reduce the H adsorption energy (ΔG H ) and facilitates the release of H 2 molecules. [6] Besides, Pt single atoms anchored alloy catalysts (Pt/np-Co 0.85 Se single-atom catalyst (SAC)) were constructed as an efficient HER electrocatalyst.…”

Section: Introductionmentioning

confidence: 99%

Dynamic CoRu Bond Shrinkage at Atomically Dispersed Ru Sites for Alkaline Hydrogen Evolution Reaction

Zhang

Soldatov

et al. 2021

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Accurately manipulating the electronic structure of metal active sites under working conditions is central to developing efficient and stable electrocatalysts in industrial water‐alkali electrolyzers. However, the lack of an intuitive means to capture the evolution of metal sites during the reaction state inhibits the manipulation of its electronic structure. Here, atomically dispersed Ru single‐sites on cobalt nanoparticles confined onto macro‐microporous frameworks (M‐Co NPs@Ru SAs/NC) with tunable electron coupling effect for efficient catalysis of alkaline hydrogen evolution reaction (HER) are constructed. Using operando X‐ray absorption and infrared spectroscopies, a dynamic CoRu bond shrinkage with strong electron coupling effect under working conditions is identified, which significantly promotes the adsorption of water molecules and then accelerates its dissociation to form the key H* over Ru sites for high HER activity. The well‐designed M‐Co NPs@Ru SAs/NC delivers efficient HER performance with a small overpotential of 34 mV at 10 mA cm−2 and a high turnover frequency of ≈4284 H2 h−1 at −0.05 V, 40 times higher than that of the benchmark Pt/C. This work provides a new point of view to manipulate the electronic structure of the metal active sites for highly effective electrocatalysis processes.

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Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Cited by 409 publications

References 78 publications

Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

Electronic Modulation Caused by Interfacial Ni‐O‐M (M=Ru, Ir, Pd) Bonding for Accelerating Hydrogen Evolution Kinetics

Dynamic CoRu Bond Shrinkage at Atomically Dispersed Ru Sites for Alkaline Hydrogen Evolution Reaction

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