Asymmetric synthesis of β-amino acid derivatives by stereocontrolled C(sp3)-C(sp2) cross-electrophile coupling via radical 1,2-nitrogen migration DOI Creative Commons
Shi Tang,

Zi-Cheng Liao,

Mengwu Xiao

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 26, 2024

Abstract Optically pure non-natural β-amino acids are noteworthy molecular motifs of numerous pharmaceutically important molecules. Skeletal editing abundant α-amino acid scaffolds via tandem radical 1,2-N-shift/cross-coupling represents an attractive and powerful tool to straightforward assemble new molecules; however, this strategy presents substantial challenges owing difficulties in reactivity regio-/enantiocontrol. Herein, we report unprecedented remote cross-electrophile C(sp2)-C(sp3) coupling β-bromo esters with aryl bromides a π-system-independent 1,2-N-shift, which allows access α-arylated β-amino high efficiency regioselectivity. Furthermore, upon the novel cooperative catalysis Ni(II)/new-style Box complex chiral phosphoric (CPA), migratory further achieves enantioselectivity control C(sp3)–C(sp2) bond construction. In addition, detailed experimental studies DFT calculations were conducted gain insight into mechanism origin enantioselectivity, was evidenced by two-step synthesis pan-Akt inhibitor molecule. Overall, synergistic expands these methods challenging enantioselective C(sp2)–C(sp3) 1,2-amino migration.

Language: Английский

Optimal Electrocatalyst Design Strategies for Acidic Oxygen Evolution DOI Creative Commons
Dongdong Zhang, Qilong Wu, Liyun Wu

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(38)

Published: Aug. 9, 2024

Abstract Hydrogen, a clean resource with high energy density, is one of the most promising alternatives to fossil. Proton exchange membrane water electrolyzers are beneficial for hydrogen production because their current facile operation, and gas purity. However, large‐scale application electrochemical splitting acidic electrolytes severely limited by sluggish kinetics anodic reaction inadequate development corrosion‐ highly oxidation‐resistant anode catalysts. Therefore, catalysts excellent performance long‐term durability must be developed oxygen evolution reactions (OER) in media. This review comprehensively outlines three commonly employed strategies, namely, defect, phase, structure engineering, address challenges within OER, while also identifying existing limitations. Accordingly, correlation between material design strategies catalytic discussed terms contribution activity stability. In addition, various nanostructures that can effectively enhance catalyst at mesoscale summarized from perspective engineering technology, thus providing suitable satisfy industrial requirements. Finally, future outlook area OER presented.

Language: Английский

Citations

9
Proton Exchange Membrane Water Splitting: Advances in Electrode Structure and Mass‐Charge Transport Optimization DOI Creative Commons
Wenting Feng, Bin Chang, Yuanfu Ren

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Abstract Proton exchange membrane water electrolysis (PEMWE) represents a promising technology for renewable hydrogen production. However, the large‐scale commercialization of PEMWE faces challenges due to need acid oxygen evolution reaction (OER) catalysts with long‐term stability and corrosion‐resistant electrode assemblies (MEA). This review thoroughly examines deactivation mechanisms acidic OER crucial factors affecting assembly instability in complex environments, including catalyst degradation, dynamic behavior at MEA triple‐phase boundary, equipment failures. Targeted solutions are proposed, improvements, optimized designs, operational strategies. Finally, highlights perspectives on strict activity/stability evaluation standards, situ/operando characteristics, practical electrolyzer optimization. These insights emphasize interrelationship between catalysts, MEAs, activity, stability, offering new guidance accelerating systems.

Language: Английский

Citations

1
Synergistic reductive-oxidative removal of halogenated organics via photoelectrochemical activation of sulfite DOI
Ge Song,

Ruiheng Liang,

Jiayi He

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125161 - 125161

Published: Feb. 1, 2025

Language: Английский

Citations

0
Hierarchical Core-Shell Cu@Cu-Ni-Co Alloy Electrocatalyst for Efficient Hydrogen Evolution in Alkaline Media DOI Creative Commons
Hussein A. Younus, Maimouna Al Hinai, Mohammed Al‐Abri

et al.

Energies, Journal Year: 2025, Volume and Issue: 18(6), P. 1515 - 1515

Published: March 19, 2025

The development of advanced electrocatalysts plays a pivotal role in enhancing hydrogen production through water electrolysis. In this study, we employed two-step electrodeposition method to fabricate 3D porous Cu-Co-Ni alloy with superior catalytic properties and long-term stability for evolution reaction (HER). resulting trimetallic alloy, Cu@Cu-Ni-Co, demonstrated significant improvements structural integrity performance. A comparative analysis electrocatalysts, including Cu, Cu@Ni-Co, revealed that Cu@Cu-Ni-Co achieved the best results alkaline media. Electrochemical tests conducted 1.0 M NaOH showed reached current density 10 mA cm−2 at low overpotential 125 mV, along Tafel slope 79.1 mV dec−1. catalyst exceptional durability, retaining ~95% its initial after 120 h continuous operation high densities. Structural confirmed enhanced performance arises from synergistic interaction between Ni, Co within well-integrated framework. This integration large electrochemical active surface area (ECSA) 380 cm2 charge transfer resistance (15.76 Ω), facilitating efficient electron promoting HER activity. These findings position as highly stable electrocatalyst conditions.

Language: Английский

Citations

0
Phosphorus-modified Basic Nickel Silicate Derivated from Vermiculite for Efficient Oxygen Evolution Reaction DOI Creative Commons
Shengliang Zhong, Jing Gao,

Chaochao Tao

et al.

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Abstract The pursuit of clean and sustainable energy sources has intensified the research focus on water electrolysis, particularly oxygen evolution reaction (OER), which serves as a pivotal step in hydrogen generation. However, development efficient cost-effective OER catalysts remains major bottleneck hindering widespread adoption electrolysis technology. In this work, utilizing vermiculite (VMT), an abundant environmentally friendly clay mineral, was employed precursor to obtain SiO2(V-SiO2). We have successfully synthesized novel phosphate-modified layered nickel silicate Ni3Si2O5(OH)4 (NiSi-P) derived from VMT through combination hydrothermal vapor deposition method. Electrochemical evaluations 1.0 M KOH revealed that NiSi-P exhibited remarkable performance, achieving low overpotential 334 mV at 10 mA·cm-2, significantly outperforming unmodified (NiSi, 564 mV). This improvement is attributed unique structural features surface chemistry NiSi-P, facilitate charge transfer protonation/deprotonation during catalytic process. study provided idea for application low-cost materials electrocatalytic splitting OER.

Language: Английский

Citations

0
Recent Advances of Ruthenium‐Based Electrocatalysts for Industrial Water Electrolyzers DOI
Wentao Zhou,

Chen Gu,

Lingbin Xie

et al.

Advanced Sustainable Systems, Journal Year: 2025, Volume and Issue: unknown

Published: April 10, 2025

Abstract Hydrogen production by electrochemical water splitting is considered to be a key strategic energy technology, and proton exchange membrane electrolyzers (PEMWEs) anion (AEMWEs) are ideal technologies for green hydrogen in recent years. However, PEMWEs AEMWEs lack low‐cost high‐performance acidic oxygen evolution reaction (OER) alkaline (HER) electrocatalysts respectively, limiting their large‐scale development. Recently, ruthenium (Ru)‐based have received lot of attention because activity better than that commercial catalysts price more affordable, showing great potential OER HER. there still obstacles Ru‐based practical applications industrial electrolyzers, regulatory strategies need developed further optimize its performance. Herein, comprehensive review presented concerning it. First, fundamental principles focus the basic content application discussed. Then, summarized, providing detailed analysis elucidate mechanisms, properties, electrolyzers. Finally, outlooks prospects challenges future proposed.

Language: Английский

Citations

0
Thiophene-functionalized triazolate metal-organic frameworks for enhanced oxygen evolution reaction: Insights from electrochemical studies and DFT calculations DOI
Limin Ma, Muhammad Imran Anwar, Faheem Abbas

et al.

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 127, P. 447 - 461

Published: April 15, 2025

Language: Английский

Citations

0
Ultrafine CoFe Alloy Nanoparticles Confined in Highly Ordered Mesoporous Carbon Films as Catalysts for the Oxygen Evolution Reaction DOI

Yi Hua Zhou,

Yanna Guo, Yusuke Yamauchi

et al.

ACS Applied Nano Materials, Journal Year: 2024, Volume and Issue: 7(22), P. 25360 - 25368

Published: Nov. 11, 2024

Thin carbon films with two different kinds of mesoporous structures (three-dimensional (3D) cubic and two-dimensional (2D) hexagonal) loaded CoFe alloy nanoparticles have been successfully synthesized by a dip-coating method high-temperature calcination under N2 atmosphere. Ultrafine bimetallic are introduced into these types as electrochemically active sites. Comparable experiments indicate that the 3D film embedded ultrafine exhibites larger electrochemical surface area lower charge transfer impedance compared 2D hexagonal supporting material. This material shows superior catalytic performance for oxygen evolution reaction (OER) overpotential (η10) 366 mV (j = 10 mA cm–2), outperforming (386 mV) at same current density.

Language: Английский

Citations

1
Asymmetric synthesis of β-amino acid derivatives by stereocontrolled C(sp3)-C(sp2) cross-electrophile coupling via radical 1,2-nitrogen migration DOI Creative Commons
Shi Tang,

Zi-Cheng Liao,

Mengwu Xiao

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 26, 2024

Abstract Optically pure non-natural β-amino acids are noteworthy molecular motifs of numerous pharmaceutically important molecules. Skeletal editing abundant α-amino acid scaffolds via tandem radical 1,2-N-shift/cross-coupling represents an attractive and powerful tool to straightforward assemble new molecules; however, this strategy presents substantial challenges owing difficulties in reactivity regio-/enantiocontrol. Herein, we report unprecedented remote cross-electrophile C(sp2)-C(sp3) coupling β-bromo esters with aryl bromides a π-system-independent 1,2-N-shift, which allows access α-arylated β-amino high efficiency regioselectivity. Furthermore, upon the novel cooperative catalysis Ni(II)/new-style Box complex chiral phosphoric (CPA), migratory further achieves enantioselectivity control C(sp3)–C(sp2) bond construction. In addition, detailed experimental studies DFT calculations were conducted gain insight into mechanism origin enantioselectivity, was evidenced by two-step synthesis pan-Akt inhibitor molecule. Overall, synergistic expands these methods challenging enantioselective C(sp2)–C(sp3) 1,2-amino migration.

Language: Английский

Citations

0