Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

Yao, Yancai; Hu, Sulei; Chen, Wenxing; Huang, Zheng-Qing; Wei, Weichen; Yao, Takeshi; Liu, Ruirui; Zang, Ketao; Wang, Xiaoqian; Wu, Geng; Yuan, Wenjuan; Yuan, Tongwei; Zhu, Bai-Quan; Liu, Wei; Li, Zhijun; He, Dongsheng; Xue, Zhenggang; Wang, Yu; Zheng, Xusheng; Dong, Juncai; Chang, Chun‐Ran; Chen, Yanxia; Hong, Xun; Luo, Jun; Wei, Shiqiang; Li, Wei‐Xue; Strasser, Peter; Wu, Yuen; Li, Yadong

doi:10.1038/s41929-019-0246-2

Cited by 800 publications

(537 citation statements)

References 53 publications

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“…162,[165][166][167][168][169][170] To improve atom utilization, Yao et al recently reported engineering the electronic structure of single-atom Ru sites via compressive strain to boost water oxidation in an acidic medium. 171 Although such a strategy of a single-atom catalyst offers one direction for catalyst design toward practical application in an acidic medium, it is still imperative and a great challenge to develop efficient and stable nonprecious OER catalysts in acidic medium.…”

Section: Development Of An Anion Exchange Membrane Alkaline Electrolymentioning

confidence: 99%

Strategies to Break the Scaling Relation toward Enhanced Oxygen Electrocatalysis

Huang

Song

Dou

et al. 2019

Matter

337

297

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The vision of a hydrogen economy relies on efficient utilization and production of hydrogen in a hydrogen fuel cell and a water electrolyzer. In both technologies, the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) account for the most efficiency loss because the reactions on catalytic sites are constrained by adsorption-energy scaling relations involving intermediates of *OOH, *O, and *OH (where * denotes the active site). Therefore, a novel paradigm for catalyst design is required by overcoming or circumventing the adsorption-energy scaling relations. In this Review, the fundamentals of oxygen electrocatalysis, including reaction of the mechanism and origin of the adsorption-energy scaling relationship, are first introduced. Crucial strategies to overcome the scaling relations are then summarized. Finally, future research directions in this area are proposed. This work provides guidelines for the rational design of efficient catalysts for oxygen electrocatalysis beyond the limitation posed by scaling relations.

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Section: Development Of An Anion Exchange Membrane Alkaline Electrolymentioning

confidence: 99%

Strategies to Break the Scaling Relation toward Enhanced Oxygen Electrocatalysis

Huang

Song

Dou

et al. 2019

Matter

337

297

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“…[11] Recent findings show that adjusting the latticestrain in catalysts can enhance their catalytic activity. [12] The intercalation of ions into electrode materials such as graphite or transition-metal dichalcogenides has proven to be an accessible way to introduce ac ontrollable level of strain and therefore tune the catalytic activity of certain catalysts. [13] The positive impact of the strain on the catalytic activity of certain materials can be traced back to ashift of the binding energy of adsorbates towards the optimum.…”

Section: Introductionmentioning

confidence: 99%

Advanced Bifunctional Oxygen Reduction and Evolution Electrocatalyst Derived from Surface‐Mounted Metal–Organic Frameworks

et al. 2020

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Metal–organic frameworks (MOFs) and their derivatives are considered as promising catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), which are important for many energy provision technologies, such as electrolyzers, fuel cells and some types of advanced batteries. In this work, a “strain modulation” approach has been applied through the use of surface‐mounted NiFe‐MOFs in order to design an advanced bifunctional ORR/OER electrocatalyst. The material exhibits an excellent OER activity in alkaline media, reaching an industrially relevant current density of 200 mA cm−2 at an overpotential of only ≈210 mV. It demonstrates operational long‐term stability even at a high current density of 500 mA cm−2 and exhibits the so far narrowest “overpotential window” ΔEORR‐OER of 0.69 V in 0.1 m KOH with a mass loading being two orders of magnitude lower than that of benchmark electrocatalysts.

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“…While the uncertainty associated with the calculation of ΔG HOO Ã À ΔG HO Ã can reduce that overpotential wall (see Supplementary Fig. 6 and Supplementary Note 3 for a detailed discussion) 15 , as has been experimentally observed for a few exceptional OER electrocatalysts [16][17][18][19][20][21] , hurdling or reducing this wall remains a major challenge.…”

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confidence: 99%

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential

et al. 2019

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A major roadblock in realizing large-scale production of hydrogen via electrochemical water splitting is the cost and inefficiency of current catalysts for the oxygen evolution reaction (OER). Computational research has driven important developments in understanding and designing heterogeneous OER catalysts using linear scaling relationships derived from computed binding energies. Herein, we interrogate 17 of the most active molecular OER catalysts, based on different transition metals (Ru, Mn, Fe, Co, Ni, and Cu), and show they obey similar scaling relations to those established for heterogeneous systems. However, we find that the conventional OER descriptor underestimates the activity for very active OER complexes as the standard approach neglects a crucial one-electron oxidation that many molecular catalysts undergo prior to O-O bond formation. Importantly, this additional step allows certain molecular catalysts to circumvent the "overpotential wall", leading to enhanced performance. With this knowledge, we establish fundamental principles for the design of ideal molecular OER catalysts.

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Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis

Cited by 800 publications

References 53 publications

Strategies to Break the Scaling Relation toward Enhanced Oxygen Electrocatalysis

Strategies to Break the Scaling Relation toward Enhanced Oxygen Electrocatalysis

Advanced Bifunctional Oxygen Reduction and Evolution Electrocatalyst Derived from Surface‐Mounted Metal–Organic Frameworks

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential

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