Controlling the Valence‐Electron Arrangement of Nickel Active Centers for Efficient Hydrogen Oxidation Electrocatalysis

Zhao, Xu; Li, Xiangyang; An, Liwei; Zheng, Lirong; Yang, Jinlong; Wang, Deli

doi:10.1002/anie.202206588

Cited by 34 publications

(28 citation statements)

References 37 publications

(45 reference statements)

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“…[ 8 ] Clearly, developing highly active, CO‐tolerant Pt‐free catalysts for alkaline HOR is industrially important. [ 21–23 ]…”

Section: Introductionmentioning

confidence: 99%

“…[8] Clearly, developing highly active, CO-tolerant Pt-free catalysts for alkaline HOR is industrially important. [21][22][23] Among Pt-free HOR catalysts developed, ruthenium (Ru) has received much attention due to similar electronic structure to that of Pt, much lower cost (approximately 50% of Pt price), and significantly higher CO tolerance. [24,25] To boost the catalytic activity and CO tolerance of Ru-based catalysts for alkaline HOR, the previous studies have focused on controlling and optimizing the surface and interface chemistry via engineering the size, composition, surface structure, and support.…”

Section: Introductionmentioning

confidence: 99%

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Tailoring Interfacial Chemistry of Defective Carbon‐Supported Ru Catalyst Toward Efficient and CO‐Tolerant Alkaline Hydrogen Oxidation Reaction

Yang

Lai

et al. 2023

Advanced Energy Materials

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The ability to create highly active and CO-tolerant platinum-free catalysts toward alkaline hydrogen oxidation reaction (HOR) represents a significant endeavor to enable commercialization of alkaline fuel cells. This, however, remains a grand challenge. Herein, a robust defective-carbon-supported Ru catalyst (denoted as Ru@C) is crafted to achieve efficient and CO-tolerant HOR in alkaline media via delicately tailoring interfacial chemistry of catalyst. Notably, the degree of defects in the carbon support is the key to tune the interface chemistry. An integrated experimental and density functional theory calculations study demonstrates that the favorable interfacial chemical interaction between Ru and carbon support controlled by the covalently bonded Ru─O─C redistributes the d electrons of Ru and downshiftsits d-band center, which in turn weakens the hydrogen adsorption and suppresses the Ru 4d→CO 2𝝅* back donation. Consequently, the optimized Ru@C catalyst renders a 6.6-fold enhancement in mass activity (@25 mV) for alkaline HOR over the conventional Ru/C counterpart, which also outperforms the state-of-the-art catalysts. Intriguingly, the catalyst can tolerate 20 000 ppm CO, far exceeding that of commercial Pt/C and PtRu/C catalysts. This work elucidates the correlation between precisely tailored interfacial chemistry and HOR performance, and is expected to further enlighten the design of advanced catalysts.

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“…[ 8 ] Clearly, developing highly active, CO‐tolerant Pt‐free catalysts for alkaline HOR is industrially important. [ 21–23 ]…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Tailoring Interfacial Chemistry of Defective Carbon‐Supported Ru Catalyst Toward Efficient and CO‐Tolerant Alkaline Hydrogen Oxidation Reaction

Yang

Lai

et al. 2023

Advanced Energy Materials

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“…As the valance electron density could manipulate bond strength and adsorption behavior, properly reducing the electron density of Ni sites might be a promising strategy for accelerating the HOR kinetics. Wang's group fabricated a series of Ni 3 N nanosheets with different deficiency proportion for optimizing charge distribution condition [26] . Among them, Ni 3 N nanosheets with enriched Ni vacancies (Ni 3 N‐r) showed the best intrinsic activity.…”

Section: Strategies For Enhancing the Alkaline Hor Activities Of Ni‐b...mentioning

confidence: 99%

Nickel‐Based Electrocatalysts for Hydrogen Oxidation Reaction Under Alkaline Electrolytes

Jin

Jia

et al. 2023

ChemCatChem

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Developing highly efficient and cost effective electrocatalysts towards hydrogen oxidation reaction under alkaline electrolyte is essential for the commercial application of anion exchange membrane fuel cells (AEMFCs). Nickel-based materials showed great performance for alkaline HOR which have been regarded as promising alternatives for Pt-group metals. In this review, several effective strategies which can successfully optimize the interaction with intermediates and promote the HOR kinetics of Ni under alkaline medium are discussed, including heteroatom doping, forming alloys and compounds, decorating with supports and constructing heterointerfaces. Meanwhile, based on the structural adjustment, the durabilities of Ni-based materials are enhanced significantly. We believe this paper might provide guidance for future catalysts design and mechanism investigation for alkaline HOR.

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“…Regrettably, their practical applications are severely limited by the scarcity, soaring cost, and inferior electrochemical stability of these noble metals . To overcome the dependence on noble metals, two primary approaches have been developed: developing noble-metal-free HER/HOR catalysts , or minimizing the amount of noble metal used while maintaining a superior HOR/HER performance. , …”

Section: Introductionmentioning

confidence: 99%

“…6 Regrettably, their practical applications are severely limited by the scarcity, soaring cost, and inferior electrochemical stability of these noble metals. 7 To overcome the dependence on noble metals, two primary approaches have been developed: developing noble-metal-free HER/HOR catalysts 8,9 or minimizing the amount of noble metal used while maintaining a superior HOR/HER performance. 10,11 According to the acknowledged volcano plots of the exchange current and calculated hydrogen binding energy (HBE, ΔG 0 H* ), optimal HOR electrocatalysts such as Pt present an ideal ΔG 0 H* value close to zero.…”

Section: ■ Introductionmentioning

confidence: 99%

Synergistic Regulation of Pt Clusters on Porous Support by Mo and P for Robust Bifunctional Hydrogen Electrocatalysis

et al. 2023

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Developing efficient electrocatalysts toward hydrogen oxidation and evolution reactions (HER/HOR) in alkaline electrolytes is essential for realizing renewable hydrogen technologies. Herein, we demonstrate that the introduction of dualactive species such as Mo and P (Pt/Mo,P@NC) can effectively regulate the surface electronic structure of platinum (Pt) and significantly improve the HOR/HER performance. The optimized Pt/Mo,P@NC exhibits remarkable catalytic activity, achieving a normalized exchange current density of 2.89 mA cm −2 and a mass activity of 2.3 mA μg Pt −1 , which are approximately 2.2 and 13.5 times higher than those of the state-of-the-art Pt/C catalyst, respectively. Moreover, it performs an impressive HER performance with an overpotential of 23.4 mV at 10 mA cm −2 , which is lower than most documented alkaline electrocatalysts. Experimental results reveal that the modifying effect of Mo and P optimizes the adsorption of H and OH on Pt/Mo,P@NC, resulting in an outstanding catalytic performance. This work has significant theoretical and practical significance for developing a novel and highly efficient catalyst for bifunctional hydrogen electrocatalysis.

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Controlling the Valence‐Electron Arrangement of Nickel Active Centers for Efficient Hydrogen Oxidation Electrocatalysis

Cited by 34 publications

References 37 publications

Tailoring Interfacial Chemistry of Defective Carbon‐Supported Ru Catalyst Toward Efficient and CO‐Tolerant Alkaline Hydrogen Oxidation Reaction

Tailoring Interfacial Chemistry of Defective Carbon‐Supported Ru Catalyst Toward Efficient and CO‐Tolerant Alkaline Hydrogen Oxidation Reaction

Nickel‐Based Electrocatalysts for Hydrogen Oxidation Reaction Under Alkaline Electrolytes

Synergistic Regulation of Pt Clusters on Porous Support by Mo and P for Robust Bifunctional Hydrogen Electrocatalysis

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