Machine Learning Boosted Entropy-Engineered Synthesis of CuCo Nanometric Solid Solution Alloys for Near-100% Nitrate-to-Ammonia Selectivity DOI
Yao Hu, Bo Hu, Haihui Lan

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 28, 2024

Nanometric solid solution alloys are utilized in a broad range of fields, including catalysis, energy storage, medical application, and sensor technology. Unfortunately, the synthesis these becomes increasingly challenging as disparity between metal elements grows, due to differences atomic sizes, melting points, chemical affinities. This study data-driven approach incorporating sample balancing enhancement techniques multilayer perceptron (MLP) algorithms improve model's ability handle imbalanced data, significantly boosting efficiency experimental parameter optimization. Building on this enhanced data processing framework, we developed an entropy-engineered specifically designed produce stable, nanometric copper cobalt (CuCo) alloys. Under conditions −0.425 V (vs RHE), CuCo alloy exhibited nearly 100% Faraday (FE) high ammonia production rate 232.17 mg h–1 mg–1. Stability tests simulated industrial environment showed that catalyst maintained over 80% FE exceeding 170 mg–1 testing period 120 h, outperforming most reported catalysts. To delve deeper into synergistic interaction mechanisms Cu Co, situ Raman spectroscopy was for real-time monitoring, density functional theory (DFT) calculations further substantiated our findings. These results not only highlight exceptional catalytic performance but also reflect effective electronic interactions two metals.

Language: Английский

Disentangling the Activity‐Stability Trade‐Off of Pyrrolic N‐Coordinated Fe─N4 Catalytic Sites for Long‐Life Oxygen Reduction Reaction in Acidic Medium DOI

Dongping Xue,

Shuyan Zhao, Bang‐An Lu

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(12)

Published: Jan. 8, 2024

Abstract Fe─N─C materials with Fe─N 4 sites are considered as most promising non‐precious metal‐based electrocatalysts for low‐cost proton‐exchange‐membrane fuel cells (PEMFCs). Breaking the trade‐off between activity and stability has been a long‐standing challenge in field of acidic oxygen reduction reaction (ORR). Herein, “top‐down” thermally‐driven strategy is developed to achieve highly active pyrrolic N‐coordinated Fe high spin state atomic cluster (Fe n @Fe─N pyrr ─C) discover that neighboring can synergistically stabilize such vulnerable by inhibiting their protonation. Consequently, ─C catalysts exhibit much enhanced ORR stability, endowing PEMFCs power density 804.6 mW cm −2 (testing conditions: 80 °C, 100% RH, 2.0 bar) over 100 h durability (at 0.5 V). These findings open up opportunities exploration durable other applications.

Language: Английский

Citations

17
Promoting Electrocatalytic Oxygen Reactions Using Advanced Heterostructures for Rechargeable Zinc–Air Battery Applications DOI
D.L. Qiu, Huihui Wang,

Tingting Ma

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(33), P. 21651 - 21684

Published: Aug. 12, 2024

In order to facilitate electrochemical oxygen reactions in electrically rechargeable zinc-air batteries (ZABs), there is a need develop innovative approaches for efficient electrocatalysts. Due their reliability, high energy density, material abundance, and ecofriendliness, ZABs hold promise as next-generation storage conversion devices. However, the large-scale application of currently hindered by slow kinetics reduction reaction (ORR) evolution (OER). development heterostructure-based electrocatalysts has potential surpass limitations imposed intrinsic properties single material. This Account begins with an explanation configurations fundamentals electrochemistry air electrode. Then, we summarize recent progress respect variety heterostructures that exploit bifunctional electrocatalytic overview impact on ZAB performance. The range heterointerfacial engineering strategies improving ORR/OER performance includes tailoring surface chemistry, dimensionality catalysts, interfacial charge transfer, mass transport, morphology. We highlight multicomponent design take these features into account create advanced highly active catalysts. Finally, discuss challenges future perspectives this important topic aim enhance activity batteries.

Language: Английский

Citations

16
Engineering Metal Electron Spin Polarization to Regulate p‐Band Center of Se for Enhanced Sodium‐Ion Storage DOI
Dandan Wang, Yunfeng Chao,

Kaiyang Guo

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(40)

Published: July 25, 2024

Abstract Sluggish ion diffusion of large sodium ions is one the main drawbacks challenging development metal selenides‐based anode materials for sodium‐ion batteries (SIBs). A spin‐state regulating strategy first proposed in this work to lift p‐band center (ɛ p ) Se a fast Na + transfer kinetic (Co,Cu)Se 2 . By utilizing electron from Cu Co, π‐symmetry t 2g Co fully occupied decrease spin polarization. The resultant repulsion between and weakens Co–Se bond ɛ Se. enhanced adsorption energy effectively accelerates at active material–electrolyte interface. As result, /NC electrode exhibits an superior storage performance with capacity 445 mAh g −1 0.2 , 312 50 363 after 10 000 cycles 10.0 insight into working mechanism metals can provide guidelines both material high‐performance SIBs.

Language: Английский

Citations

14
Entropy-Engineered Middle-In Synthesis of Dual Single-Atom Compounds for Nitrate Reduction Reaction DOI
Yao Hu, Haihui Lan, Junjun He

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(34), P. 23168 - 23180

Published: July 24, 2024

Despite the immense potential of Dual Single-Atom Compounds (DSACs), challenges in their synthesis process, including complexity, stability, purity, and scalability, remain primary concerns current research. Here, we present a general strategy, termed "Entropy-Engineered Middle-In Synthesis Compounds" (EEMIS-DSAC), which is meticulously crafted to produce diverse range DSACs, effectively addressing aforementioned issues. Our strategy integrates advantages both bottom-up top-down paradigms, proposing an insight into optimizing catalyst structure. The as-fabricated DSACs exhibited excellent activity stability nitrate reduction reaction (NO3RR). In significant advancement, our prototypical CuNi demonstrated outstanding performance under conditions reminiscent industrial wastewater. Specifically, NO3– concentration 2000 ppm, it yielded Faradaic efficiency (FE) for NH3 96.97%, coupled with mass productivity 131.47 mg h–1 mg–1 area 10.06 cm–2. Impressively, even heightened 0.5 M, FE peaked at 90.61%, reaching 1024.50 78.41 This work underpins EEMIS-DSAC approach, signaling frontier high-performing DSACs.

Language: Английский

Citations

9
Constructing Directional Electrostatic Potential Difference via Gradient Nitrogen Doping for Efficient Oxygen Reduction Reaction DOI
Zhijie Qi, Zhenjie Lu,

Xiangjie Guo

et al.

Small, Journal Year: 2024, Volume and Issue: 20(34)

Published: April 9, 2024

Abstract Nitrogen doping has been recognized as an important strategy to enhance the oxygen reduction reaction (ORR) activity of carbon‐encapsulated transition metal catalysts (TM@C). However, previous reports on nitrogen have tended result in a random distribution atoms, which leads disordered electrostatic potential differences surface carbon layers, limiting further control over materials' electronic structure. Herein, gradient prepare nitrogen‐deficient graphene and nitrogen‐rich nanotubes encapsulated cobalt nanoparticles (Co@CNTs@NG) is proposed. The unique gradual increase layer from region region, facilitating directed electron transfer within these layers ultimately optimizing charge material. Therefore, this effectively regulates density state work function material, adsorption oxygen‐containing intermediates enhancing ORR activity. Theoretical experimental results show that under controlled doping, Co@CNTs@NG exhibits significantly performance (E onset = 0.96 V, E 1/2 0.86 V). At same time, also displays excellent cathode material for Zn–air batteries, with peak power 132.65 mA cm −2 open‐circuit voltage (OCV) 1.51 V. This provides effective optimize performance.

Language: Английский

Citations

8
OH‐Induced Surface Reconstitution in Single Atoms and Clusters Integrated Electrocatalysts for Self‐Adaptive Oxygen Electrocatalysis DOI
Jiawei Qi,

Litao Yu,

He Gan

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(52)

Published: Aug. 27, 2024

Abstract The integration of atom clusters and single atoms into a unified system represents desirable approach for attaining enhanced catalytic performance. Nonetheless, the controllable synthesis single‐atom nanocluster integrated (SA‐NC) faces considerable challenges, mechanisms underlying activity remain poorly understood. In this research, cobalt‐based catalyst containing both coordinatively unsaturated (CoN 3 ) small nanoclusters (Co@SA‐NC) is synthesized. Co@SA‐NC not only facilitates charge mass transfer due to interconnected long‐range micromorphology, thus endowing efficient oxygen electrocatalytic reaction (ORR/OER), but also undergoes surface reconfiguration upon OH adsorption at high potentials in alkaline ORR/OER conditions. More appealingly, OH‐involved reconfigured adaptive structure promotes optimization energy barriers owing dynamic regulation from bridged between Co cluster whole process. Specific application metrics, zinc–air battery assembled using exhibit targeted power density enhancement with 270 mW cm −2 an medium. This work offers effective insight study SA‐NC pathways catalysis.

Language: Английский

Citations

7
Activating Ru nanoclusters for robust oxygen reduction in aqueous wide-temperature zinc-air batteries DOI

Rupeng Liu,

Chunhuan Jiang,

Jin-Han Guo

et al.

Matter, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 1, 2024

Language: Английский

Citations

7
Exploring the role of iron in Fe5Ni4S8 toward oxygen evolution through modulation of electronic orbital occupancy DOI
Zhengyan Du, Zeshuo Meng,

Haoteng Sun

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 92, P. 52 - 62

Published: Jan. 24, 2024

Language: Английский

Citations

6
Synergizing Single-Atom and Carbon-Encapsulated Nanoparticles of Fe for Efficient Oxygen Reduction and Durable Zn–Air Batteries DOI
Wuyi Zhang, Chuangwei Liu, Anthony Kucernak

et al.

ACS Applied Energy Materials, Journal Year: 2024, Volume and Issue: 7(13), P. 5398 - 5407

Published: June 13, 2024

Overcoming the sluggish kinetics of oxygen reduction reaction (ORR) remains a critical challenge for Zn–air batteries. Fe–N/C catalysts have emerged as promising alternatives to precious Pt-based materials. Herein, we report design and synthesis carbon-encapsulated Fe nanoparticles decorated (denoted FeNPs@Fe–N/C) via controlled pyrolysis. The FeNPs@Fe–N/C catalyst exhibits excellent ORR performance in alkaline media with half-wave potential (E1/2) 0.893 VRHE. strategic integration substantially improves catalytic activity catalysts. battery cathode delivers an impressive peak power density 175.7 mW cm–2 stability over 500 h, surpassing Pt/C benchmarks. Density functional theory calculations reveal that facilitate electron transfer site by modulating d-band center, thereby boosting activity. This research paves way future strategies integrating single atoms efficient electrocatalysis.

Language: Английский

Citations

5
Electron Spin Polarization in Rechargeable Batteries: Theoretical Foundation and Practical Applications DOI
Huicong Xia, Yao Hu, Z. Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 9, 2024

Abstract Electron spin polarization (ESP) refers to the alignment of electron spins in a specified direction, with burgeoning research underscoring its pivotal role enhancing rechargeable batteries. This review delves into theoretical underpinnings ESP and intricate connection performance batteries, elucidating potential augment charge/discharge efficiency, elevate energy density, refine overall battery functionality. The further encompasses an overview experimental methodologies employed probe systems, spotlighting seminal discoveries from contemporary studies evaluating hurdles prospects linked practical applications. profound advantages for batteries are underscored, suggesting that harnessing this phenomenon can empower researchers engineers develop superior storage capacities, swifter charging rates, extended cycle lifespans. Such advancements expedite adoption electric vehicles seamless integration renewable sources power grids, among other high‐energy‐demand In conclusion, offers invaluable perspectives on through lens ESP, insights presented here expected catalyze innovation sector, thereby advancing development sustainable efficient technologies.

Language: Английский

Citations

5