Confined cobalt single‐atom catalysts with strong electronic metal‐support interactions based on a biomimetic self‐assembly strategy DOI Creative Commons
Bowen Guo, Zekun Wang, Lei Zheng

et al.

Carbon Energy, Journal Year: 2024, Volume and Issue: 6(9)

Published: April 17, 2024

Abstract Designing high‐performance and low‐cost electrocatalysts for oxygen evolution reaction (OER) is critical the conversion storage of sustainable energy technologies. Inspired by biomineralization process, we utilized phosphorylation sites collagen molecules to combine with cobalt‐based mononuclear precursors at molecular level built a three‐dimensional (3D) porous hierarchical material through bottom‐up biomimetic self‐assembly strategy obtain single‐atom catalysts confined on carbonized self‐assembled carriers (Co SACs/cBSC) after subsequent high‐temperature annealing. In this strategy, biomolecule improved anchoring efficiency metal precursor precise functional groups; meanwhile, binding‐then‐assembling also effectively suppressed nonspecific adsorption ions, ultimately preventing atomic agglomeration achieving strong electronic metal‐support interactions (EMSIs). Experimental characterizations confirm that binding forms between cobalt substrate (Co–O 4 –P). Theoretical calculations disclose local environment changes significantly tailored Co d‐band center, optimized oxygenated intermediates barrier release. As result, obtained SACs/cBSC catalyst can achieve remarkable OER activity 24 h durability in 1 M KOH ( η 10 288 mV; Tafel slope 44 mV dec −1 ), better than other transition metal‐based commercial IrO 2 . Overall, presented prepare SACs EMSIs, providing new avenue preparation efficient fine structures.

Language: Английский

Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance DOI
Runze Li, Jie Zhao, Baozhong Liu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Oct. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Language: Английский

Citations

60
Single‐Atom Nanozymes for Catalytic Therapy: Recent Advances and Challenges DOI

Weiyi He,

Jiahao Wu, Jianli Liu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(16)

Published: Jan. 4, 2024

Abstract As a powerful tool, nanozyme catalysts broaden the avenues to implement bio‐inspired solutions for addressing many important concerns, covering energy, healthcare, environment, and more. Recent endeavors, characterized by atomic precision, have enabled extensive exploration of single‐atom nanozymes (SAzymes) with high catalytic activity, superior substrate selectivity, integrated multifunctionalities, thus becoming an emerging field that bridges nanotechnology biology. This review provides brief outline progress summarizes latest research advances regarding SAzymes in biomedical therapeutics, mainly including tumor therapy, wound antibacterial tissue anti‐inflammatory focus on their prototypical synthesis therapeutic mechanisms. Finally, current challenges future perspectives engineering advanced are also discussed outlooked. It is anticipated this area shall provide useful guidance therapy.

Language: Английский

Citations

59
Reactive Template-Engaged Synthesis of NiSx/MoS2 Nanosheets Decorated on Hollow and Porous Carbon Microtubes with Optimal Electronic Modulation toward High-Performance Enzyme-like Performance DOI

Xiaoying He,

Songbo Xie,

Jingli Xu

et al.

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(20), P. 8033 - 8042

Published: May 8, 2023

As a promising cost-effective nanozyme, MoS2 nanosheets (NSs) have been considered as good candidate for the enzyme-like catalysis. However, their catalytic activity is still restricted by insufficient active sites and poor conductivity, thus, comprehensive performances are unsatisfactory. To address these issues, herein, we design fabricate an intelligent tubular nanostructure of hierarchical hollow nanotubes, which assembled NiSx/MoS2 NSs encapsulated into N-doped carbon microtubes (NiSx/MoS2@NCMTs). The (NCMTs) serve conductive skeleton, integrating with ensuring well-distribution, thereby maximally exposing more sites. Additionally, tube-like structure favorable increasing mass transfusion to ensure excellent performance. Profiting from component structural advantages, obtained NiSx/MoS2@NCMTs exhibit surprisingly enhanced activity. Based on these, facile colorimetric sensing platform detect H2O2 GSH has developed. This proposed approach can be expected synthesize series heterostructured MoS2-based composites, will widely applied in catalysis, energy storage, disease diagnosis, etc.

Language: Английский

Citations

53
Electrochemical exfoliation of 2D materials beyond graphene DOI Creative Commons
Minghao Zhao, Cinzia Casiraghi, Khaled Parvez

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(6), P. 3036 - 3064

Published: Jan. 1, 2024

After the discovery of graphene in 2004, field atomically thin crystals has exploded with thousands 2-dimensional materials (2DMs) unique electronic and optical properties, by making them very attractive for a broad range applications, from electronics to energy storage harvesting, sensing biomedical applications. In order integrate 2DMs into practical it is crucial develop mass scalable techniques providing high quality large yield. Electrochemical exfoliation one most promising methods producing 2DMs, as enables quick large-scale production solution processable nanosheets thickness well below 10 layers lateral size above 1 μm. Originally, this technique was developed graphene; however, last few years, approach been successfully extended other such transition metal dichalcogenides, black phosphorous, hexagonal boron nitride, MXenes many emerging 2D materials. This review first provides an introduction fundamentals electrochemical then discusses each class introducing their properties giving examples Finally, summary perspective are given address some challenges research area.

Language: Английский

Citations

43
Metal-Free Highly Stable and Crystalline Covalent Organic Nanosheet for Visible-Light-Driven Selective Solar Fuel Production in Aqueous Medium DOI
Sandip Biswas, Anupam Dey, Faruk Ahamed Rahimi

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(9), P. 5926 - 5937

Published: April 17, 2023

Conversion of CO2 into solar fuels via artificial photosynthesis is one the most promising and sustainable approaches to mitigate global warming worldwide energy shortage. Covalent organic frameworks (COFs) exhibit well-defined arrangements building blocks, tunable porosity, high thermal chemical stability in harsh conditions. The band gaps COFs by suitably introducing chromophoric light-harvesting units make them a unique class metal-free heterogeneous photocatalysts for successful conversion fuel. In this work, we report simple, efficient, low-cost 2D COF (TTA-Tz) composed 1,3,5-tris-(4-aminophenyl)triazine (TTA) 4,4′-(thiazolo[5,4-d]thiazole-2,5-diyl)dibenzaldehyde (Tz) photocatalytic reduction. 2D-layered exfoliated ultrathin covalent nanosheets (CONs), which shows visible-light-driven photoreduction CO (yield = 2.8 mmol g–1, rate 82 μmol h–1 selectivity >99%) aqueous medium without an external sacrificial electron donor. Interestingly, mixed solvent system, evolution (163 g–1 h–1) found double than case with 99% selectivity. By both BNAH TEA as donors, significant amount CH4 (499 g–1) produced (310 further enhanced. mechanistic insight reduction studied DFT-based theoretical calculation, supported situ diffuse reflectance spectroscopy study.

Language: Английский

Citations

42
Phase Engineering of Nanomaterials: Transition Metal Dichalcogenides DOI
Wei Zhai, Zijian Li, Yongji Wang

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(7), P. 4479 - 4539

Published: March 29, 2024

Crystal phase, a critical structural characteristic beyond the morphology, size, dimension, facet, etc., determines physicochemical properties of nanomaterials. As group layered nanomaterials with polymorphs, transition metal dichalcogenides (TMDs) have attracted intensive research attention due to their phase-dependent properties. Therefore, great efforts been devoted phase engineering TMDs synthesize controlled phases, especially unconventional/metastable for various applications in electronics, optoelectronics, catalysis, biomedicine, energy storage and conversion, ferroelectrics. Considering significant progress synthesis TMDs, we believe that comprehensive review on is promote fundamental studies practical applications. This Review aims provide introduction discussion crystal structures, synthetic strategies, TMDs. Finally, our perspectives challenges opportunities will also be discussed.

Language: Английский

Citations

37
Electrochemistry of 2D-materials for the remediation of environmental pollutants and alternative energy storage/conversion materials and devices, a comprehensive review DOI
Saleem Raza, Asif Hayat, Tariq Bashir

et al.

Sustainable materials and technologies, Journal Year: 2024, Volume and Issue: 40, P. e00963 - e00963

Published: May 8, 2024

Language: Английский

Citations

33
Asymmetric Atomic Dual‐Sites for Photocatalytic CO2 Reduction DOI Creative Commons
Guangri Jia,

Yingchuan Zhang,

Jimmy C. Yu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

Citations

29
Single‐Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis DOI

Xin‐Yu Wang,

Yong‐Zhou Pan,

Jiarui Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single-electron transfer on electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, problems this chemistry still exist such as dosage, difficult recovery, and low efficiency. Single-atom catalysts (SACs) exhibit atom utilization excellent activity, hold great promise in addressing limitations homogeneous catalysts. In view this, we have employed Fe-SA@NC an advanced redox mediator to try change situation. was synthesized using encapsulation-pyrolysis method, it demonstrated remarkable performance a range reported reactions, construction various C-C/C-X bonds. Moreover, potential exploring new synthetic method for electrosynthesis. We develop electro-oxidative ring-opening transformation cyclopropyl amides. reaction system, showed good tolerance drug molecules with complex structures, well flow electrochemical syntheses gram-scale transformations. This work highlights SACs electrosynthesis, thereby opening avenue chemistry.

Language: Английский

Citations

28
Challenges and Opportunities for Single‐Atom Electrocatalysts: From Lab‐Scale Research to Potential Industry‐Level Applications DOI Creative Commons
Chen Jia, Qian Sun, Ruirui Liu

et al.

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

Published: June 13, 2024

Single-atom electrocatalysts (SACs) are a class of promising materials for driving electrochemical energy conversion reactions due to their intrinsic advantages, including maximum metal utilization, well-defined active structures, and strong interface effects. However, SACs have not reached full commercialization broad industrial applications. This review summarizes recent research achievements in the design crucial electrocatalytic on sites, coordination, substrates, as well synthesis methods. The key challenges facing activity, selectivity, stability, scalability, highlighted. Furthermore, it is pointed out new strategies address these increasing activity enhancing utilization improving optimizing local environment, developing fabrication techniques, leveraging insights from theoretical studies, expanding potential Finally, views offered future direction single-atom electrocatalysis toward commercialization.

Language: Английский

Citations

26