First principle investigation of W/P3C sheet as an efficient single atom electrocatalyst for N2 and NO electrochemical reaction with suppressed hydrogen evolution

AbstractTuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.

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Identifying the Activity Origin of a Cobalt Single‐Atom Catalyst for Hydrogen Evolution Using Supervised Learning

Advanced Functional Materials ◽

10.1002/adfm.202100547 ◽

2021 ◽

pp. 2100547

Author(s):

Xinghui Liu ◽

Lirong Zheng ◽

Chenxu Han ◽

Hongxiang Zong ◽

Guang Yang ◽

...

Keyword(s):

Supervised Learning ◽

Hydrogen Evolution ◽

Single Atom

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Ultralow Loading (Single‐Atom and Clusters) of the Pt Catalyst by Atomic Layer Deposition Using Dimethyl ((3,4‐η) N , N ‐dimethyl‐3‐butene‐1‐amine‐ N ) Platinum (DDAP) on the High‐Surface‐Area Substrate for Hydrogen Evolution Reaction

Advanced Materials Interfaces ◽

10.1002/admi.202001508 ◽

2020 ◽

pp. 2001508

Author(s):

Rahul Ramesh ◽

Seungmin Han ◽

Dip K. Nandi ◽

Sandesh Y. Sawant ◽

Deok Hyun Kim ◽

...

Keyword(s):

Atomic Layer Deposition ◽

Surface Area ◽

Hydrogen Evolution ◽

Hydrogen Evolution Reaction ◽

High Surface ◽

High Surface Area ◽

Atomic Layer ◽

Single Atom ◽

Pt Catalyst ◽

Layer Deposition

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Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

Nano-Micro Letters ◽

10.1007/s40820-021-00679-3 ◽

2021 ◽

Vol 13 (1) ◽

Author(s):

Yingjie Yang ◽

Yanhui Yu ◽

Jing Li ◽

Qingrong Chen ◽

Yanlian Du ◽

...

Keyword(s):

Hydrogen Evolution ◽

Hydrogen Evolution Reaction ◽

Rational Design ◽

Energy System ◽

Structure Design ◽

Single Atom ◽

Research Progress ◽

Pure Hydrogen ◽

Hydrogen Energy ◽

Practical Applications

AbstractThe 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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First-principle calculations on the structure, electronic property and catalytic activity for hydrogen evolution reaction of 2D transition-metal borides

Materials Chemistry and Physics ◽

10.1016/j.matchemphys.2020.123334 ◽

2020 ◽

Vol 253 ◽

pp. 123334

Author(s):

Xin Liu ◽

Xiaoli Ge ◽

Yao Dong ◽

Kun Fu ◽

Fanbin Meng ◽

...

Keyword(s):

Catalytic Activity ◽

Transition Metal ◽

Hydrogen Evolution ◽

Hydrogen Evolution Reaction ◽

Electronic Property ◽

First Principle ◽

First Principle Calculations ◽

Metal Borides

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Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

Nature Communications ◽

10.1038/s41467-021-24828-9 ◽

2021 ◽

Vol 12 (1) ◽

Author(s):

Panlong Zhai ◽

Mingyue Xia ◽

Yunzhen Wu ◽

Guanghui Zhang ◽

Junfeng Gao ◽

...

Keyword(s):

Hydrogen Evolution ◽

Water Splitting ◽

Layered Double Hydroxide ◽

Hydrogen Evolution Reaction ◽

Active Sites ◽

Density Functional ◽

Rational Design ◽

Single Atom ◽

Nickel Iron ◽

Double Hydroxide

AbstractRational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru1/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru1/D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm−2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru1/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O–O coupling at a Ru–O active site for oxygen evolution reaction. The Ru1/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts.

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