Precise Strain Tuning Boosts Electrocatalytic Hydrogen Generation DOI
Hongyu Guo, Lu Li, Yan Chen

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(32)

Published: May 30, 2023

Abstract Strain engineering has been utilized as an effective approach to regulate the binding of reaction intermediates and modify catalytic behavior on noble metal nanocatalysts. However, continuous, precise control strain for a depiction strain‐activity correlation remains challenge. Herein, Pd‐based nanooctahedrons coated with two Ir overlayers are constructed, subject different postsynthetic treatments alter amount H intercalated into Pd core achieving three surface strains ( o ‐Pd/Ir‐1.2%, ‐Pd/Ir‐1.7%, ‐Pd/Ir‐2.1% NPs). It is demonstrated that performances ‐Pd/Ir NPs display volcano‐shaped curve against toward hydrogen evolution (HER). Specifically, ‐Pd/Ir‐1.7% exhibit superior performance mass activity 9.38 A mg −1 at −0.02 V versus reversible electrode, 10.8‐ 18.8‐fold higher than those commercial Pt/C Ir/C, respectively, making it one most active HER electrocatalysts reported date. Density function theory calculations verify moderate tensile Ir(111) surfaces plays pivotal role in optimizing energy. This work highlights new strategy over nanocrystals more efficient electrocatalysis.

Language: Английский

Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt1–Pdn–(Ni,Co)(OH)x DOI
An Pei,

Ruikuan Xie,

Lihua Zhu

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 13, 2025

Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H2 generation, avoiding its costly and risky distribution issues, but this "ME-to-H2" electric conversion suffers from high voltage (energy consumption) competitive oxygen evolution reaction. Herein, we demonstrate that synergistic cofunctional Pt1Pdn/(Ni,Co)(OH)x catalyst with Pt single atoms (Pt1) Pd nanoclusters (Pdn) anchored on OH-vacancy(VOH)-rich (Ni,Co)(OH)x nanoparticles create triadic active sites, allowing methanol-enhanced low-voltage generation. For MOR, OH* preferentially adsorbed Pdn then interacts the intermediates (such as *CHO or *CHOOH) favorably neighboring Pt1 assistance of bonding surface (Ni,Co)(OH)x. The enhanced selectivity *CHOOH pathway, instead *CO, sustains MOR activity to practically current density. HER, Pt1, Pdn, OH-vacancy sites an "acid–base" microenvironment facilitate water adsorption splitting, forming H* species *OH at vacancy, promote efficient asymmetric via Tafel mechanism. triadic-site synergy opens new avenues design synthesis highly stable catalysts "on-site-on-demand" production, here facilitated by methanol.

Language: Английский

Citations

5
Fine-tuned coordination environment of Pt-Fe-Pt active site for selective heterogeneous hydrogenation of crotonaldehyde DOI
Di Zhou, Junjun Wang,

Minzhen Jian

et al.

Chem, Journal Year: 2025, Volume and Issue: unknown, P. 102380 - 102380

Published: Jan. 1, 2025

Language: Английский

Citations

3
Biogas sequestration to carbon nanofibers via tandem catalytic strategies DOI
Zhenhua Xie, Erwei Huang,

Kevin K. Turaczy

et al.

Nature Chemical Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 12, 2025

Language: Английский

Citations

2
Single‐Atom Rh on High‐Index CeO2 Facet for Highly Enhanced Catalytic CO Oxidation DOI
Jing Xu, Ying Wang, Ke Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: May 11, 2023

Reducible oxide-supported noble metal nanoparticles exhibit high activity in catalyzing many important oxidation reactions. However, atom migration under harsh reaction conditions leads to deactivation of the catalyst. Meanwhile, single-atom catalysts demonstrate enhanced stability, but often suffer from poor catalytic owing ionized surface states. In this work, we simultaneously address and stability issues by synthesizing highly active durable rhodium (Rh) through a "wrap-bake-peel" process. The pre-coated SiO2 layer during synthesis catalyst plays crucial role not only protecting CeO2 support against sintering, also donating electron weaken Ce-O bond, producing loaded Rh single atoms on exposed with high-index {210} facets. Benefiting unique electronic structure facets, more oxygen vacancies are generated along deposition electropositive atoms, leading remarkably improved performance CO oxidation.

Language: Английский

Citations

39
Precise Strain Tuning Boosts Electrocatalytic Hydrogen Generation DOI
Hongyu Guo, Lu Li, Yan Chen

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(32)

Published: May 30, 2023

Abstract Strain engineering has been utilized as an effective approach to regulate the binding of reaction intermediates and modify catalytic behavior on noble metal nanocatalysts. However, continuous, precise control strain for a depiction strain‐activity correlation remains challenge. Herein, Pd‐based nanooctahedrons coated with two Ir overlayers are constructed, subject different postsynthetic treatments alter amount H intercalated into Pd core achieving three surface strains ( o ‐Pd/Ir‐1.2%, ‐Pd/Ir‐1.7%, ‐Pd/Ir‐2.1% NPs). It is demonstrated that performances ‐Pd/Ir NPs display volcano‐shaped curve against toward hydrogen evolution (HER). Specifically, ‐Pd/Ir‐1.7% exhibit superior performance mass activity 9.38 A mg −1 at −0.02 V versus reversible electrode, 10.8‐ 18.8‐fold higher than those commercial Pt/C Ir/C, respectively, making it one most active HER electrocatalysts reported date. Density function theory calculations verify moderate tensile Ir(111) surfaces plays pivotal role in optimizing energy. This work highlights new strategy over nanocrystals more efficient electrocatalysis.

Language: Английский

Citations

36