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

General Synthesis of a Diatomic Catalyst Library via a Macrocyclic Precursor-Mediated Approach DOI
Yu‐Xiao Zhang, Shengbo Zhang, Helai Huang

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(8), P. 4819 - 4827

Published: Feb. 15, 2023

Heterogeneous catalysts containing diatomic sites are often hypothesized to have distinctive reactivity due synergistic effects, but there limited approaches that enable the convenient production of (DACs) with diverse metal combinations. Here, we present a general synthetic strategy for constructing DAC library across wide spectrum homonuclear (Fe2, Co2, Ni2, Cu2, Mn2, and Pd2) heteronuclear (Fe-Cu, Fe-Ni, Cu-Mn, Cu-Co) bimetal centers. This is based on an encapsulation-pyrolysis approach, wherein porous material-encapsulated macrocyclic complex mediates structure DACs by preserving main body molecular framework during pyrolysis. We take oxygen reduction reaction (ORR) as example show this can provide great opportunities electrocatalyst development unlocking unconventional pathway. Among all investigated sites, Fe-Cu possess exceptional high durability ORR because pairs steer elementary steps in catalytic cycle suppress troublesome Fenton-like reactions.

Language: Английский

Citations

140
Advances in heterogeneous single-cluster catalysis DOI
Xinzhe Li, Sharon Mitchell, Yiyun Fang

et al.

Nature Reviews Chemistry, Journal Year: 2023, Volume and Issue: 7(11), P. 754 - 767

Published: Oct. 9, 2023

Language: Английский

Citations

91
Carbon‐Anchored Molybdenum Oxide Nanoclusters as Efficient Catalysts for the Electrosynthesis of Ammonia and Urea DOI

Mengmiao Sun,

Guanzheng Wu,

Jiadi Jiang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)

Published: March 13, 2023

Abstract The electrochemical NO 3 − reduction and its coupling with CO 2 can provide novel clean routes to synthesize NH urea, respectively. However, their practical application is still impeded by the lack of efficient catalysts desirable Faradaic efficiency (FE) yield rate. Herein, we report synthesis molybdenum oxide nanoclusters anchored on carbon black (MoO x /C) as electrocatalyst. It affords an outstanding FE 98.14 % rate 91.63 mg h −1 cat. in reduction. Besides, highest 27.7 a maximum urea 1431.5 μg toward also achieved. formation electron‐rich MoO highly unsaturated metal sites /C heterostructure beneficial for enhanced catalytic performance. Studies mechanism reveal that stabilization *NO *CO NOOH intermediates are critical synthesis,

Language: Английский

Citations

76
Optimizing Intermediate Adsorption via Heteroatom Ensemble Effect over RuFe Bimetallic Alloy for Enhanced Nitrate Electroreduction to Ammonia DOI
Xinying Zhao, Yuzhuo Jiang, Mengfan Wang

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(31)

Published: June 30, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach for removal and NH synthesis at ambient conditions. As complex eight‐electron/nine‐proton transfer process, its performance relies heavily on the adsorption ability of intermediates catalyst surface, which determined by geometric electronic configurations active sites. In this work, heteroatom ensemble effect deliberately triggered over RuFe bimetallic alloy to optimize intermediate NO RR. A record‐high yield rate 118.8 mg h −1 high Faradaic efficiency 92.2% are achieved −1.4 V vs reversible hydrogen electrode, ranking top state‐of‐the‐art. Experimental computational results reveal that characteristics induced play crucial roles. Both Ru Fe display continuous state throughout Fermi level, suggesting electron density benefits whole result, facilitated − , efficient stabilization key intermediates, as well timely desorption simultaneously achieved, thus significantly promoting direct .

Language: Английский

Citations

73
Single Cu–N4sites enable atomic Fe clusters with high-performance oxygen reduction reactions DOI

Shuwen Wu,

Shang Jiang,

Shaoqing Liu

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(8), P. 3576 - 3586

Published: Jan. 1, 2023

Atomic Fe clusters functionalized by Cu–N 4 sites with enhanced oxygen reduction reactions (ORRs) in alkaline and acidic media.

Language: Английский

Citations

63
State-of-the-art single-atom catalysts in electrocatalysis: From fundamentals to applications DOI
Muhammad Humayun, Muhammad Israr, Abbas Khan

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 113, P. 108570 - 108570

Published: May 29, 2023

Language: Английский

Citations

57
Recent progress of manganese dioxide based electrocatalysts for the oxygen evolution reaction DOI Creative Commons

Yunlong He,

Zhenye Kang,

Jing Li

et al.

Industrial Chemistry and Materials, Journal Year: 2023, Volume and Issue: 1(3), P. 312 - 331

Published: Jan. 1, 2023

This review discusses the OER reaction mechanism (AEM and LOM) research progress of MnO 2 -based catalysts. The optimization strategy catalysts was summarized.

Language: Английский

Citations

52
Emerging Atomically Precise Metal Nanoclusters and Ultrasmall Nanoparticles for Efficient Electrochemical Energy Catalysis: Synthesis Strategies and Surface/Interface Engineering DOI
Mingjie Wu, Fang Dong, Yingkui Yang

et al.

Electrochemical Energy Reviews, Journal Year: 2024, Volume and Issue: 7(1)

Published: March 9, 2024

Language: Английский

Citations

51
Decoupling the Interfacial Catalysis of CeO2-Supported Rh Catalysts Tuned by CeO2 Morphology and Rh Particle Size in CO2 Hydrogenation DOI

Weiqi Liao,

Minnan Yue,

Junyi Chen

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(8), P. 5767 - 5779

Published: April 13, 2023

Metal–oxide interfaces play a crucial role in catalyzing CO2 conversion, while comprehensively decoupling interfacial catalysis is challenging due to their structural complexity. Herein, Rh/CeO2 catalysts, whose structures are finely tuned by altering the CeO2 morphologies and Rh particle sizes, were employed for hydrogenation. The results reveal that density of oxygen vacancies varies with determines catalytic activity, product selectivity strongly depends on nature supported species. With decrease size, weakened metallicity suppression Sabatier reaction thus low CH4 selectivity. Meanwhile, enhanced reverse water–gas shift process more easily catalyzed than contributes promotion efficiency. Interestingly, increases temperature rise at fine particles, which could be ascribed H-spillover effect high temperatures. Spectroscopic confirm hydrogenation proceeding through redox mechanism generate an adsorbed CO intermediate either further hydrogenated into strong adsorption capacity/H-spillover or desorbs directly CO.

Language: Английский

Citations

47
Collective Effect in a Multicomponent Ensemble Combining Single Atoms and Nanoparticles for Efficient and Durable Oxygen Reduction DOI

Xiaochun Xu,

Xinyi Li, Wenting Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 13, 2024

Abstract Metal single‐atom catalysts represent one of the most promising non‐noble metal for oxygen reduction reaction (ORR). However, they still suffer from insufficient activity and, particularly, durability practical applications. Leveraging density functional theory (DFT) and machine learning (ML), we unravel an unexpected collective effect between FeN 4 OH sites, CeN motifs, Fe nanoparticles (NPs), Fe−CeO 2 NPs. The comprises differently‐weighted electronic geometric interactions, whitch results in significantly enhanced ORR active sites with a half‐wave potential ( E 1/2 ) 0.948 V versus reversible hydrogen electrode (V RHE alkaline, relative to commercial Pt/C , 0.851 ). Meanwhile, this endows shortened Fe−N bonds remarkable negligible loss after 50,000 cycles. ML was used understand intricate interactions reveal intrinsic descriptors account performance. universality demonstrated effective Co, Ni, Cu, Cr, Mn‐based multicomponent ensembles. These confirm importance simultaneously improve catalytic durability.

Language: Английский

Citations

40