Understanding the Dynamic Evolution of Active Sites among Single Atoms, Clusters, and Nanoparticles DOI Open Access

Hongchen Yang,

Pengfei Duan, Zechao Zhuang

et al.

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

Published: Jan. 2, 2025

Abstract Catalysis remains a cornerstone of chemical research, with the active sites catalysts being crucial for their functionality. Identifying sites, particularly during reaction process, is elucidating relationship between catalyst's structure and its catalytic property. However, dynamic evolution within heterogeneous metal presents substantial challenge accurately pinpointing real sites. The advent in situ operando characterization techniques has illuminated path toward understanding changes offering robust scientific evidence to support rational design catalysts. There pressing need comprehensive review that systematically explores among single atoms, clusters, nanoparticles as utilizing techniques. This aims delineate effects various factors on nanoparticles. Moreover, several are elaborated emphases tracking linking them properties. Finally, it discusses challenges future perspectives identifying process advancing

Language: Английский

Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide DOI
Deming Tan, Rong Zhuang, Ruichong Chen

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)

Published: Dec. 6, 2023

Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O ) has garnered widespread attention. However, existing industrial production H is plagued by high consumption, harmful waste emission, severe safety issues, making it difficult to satisfy environmental/economic concept. Artificial photosynthesis offers viable strategy for green sustainable since uses sunlight as an source initiate reaction oxygen water produce . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons well‐defined active sites, have emerged promising photocatalysts production. This review presents nascent burgeoning area photocatalytic based on COFs. First, brief overview technology provided, followed detailed introduction principles evaluation generation. Subsequently, latest research progress judicious design COFs expounded, particular emphasis manipulating electronic structures redox sites. Finally, outlook challenges future opportunities proposed, hope stimulating further explorations novel molecular‐designed photosynthesis.

Language: Английский

Citations

85
P, K doped crystalline g-C3N4 grafted with cyano groups for efficient visible-light-driven H2O2 evolution DOI
Jinpeng Yuan, Na Tian, Zijian Zhu

et al.

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 467, P. 143379 - 143379

Published: May 9, 2023

Language: Английский

Citations

63
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

59
A Z‐Scheme Heterojunctional Photocatalyst Engineered with Spatially Separated Dual Redox Sites for Selective CO2 Reduction with Water: Insight by In Situ µs‐Transient Absorption Spectra DOI Open Access
Ling Sun, Ziqing Zhang, Ji Bian

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(21)

Published: March 6, 2023

Solar-driven CO2 reduction by water with a Z-scheme heterojunction affords an avenue to access energy storage and alleviate greenhouse gas (GHG) emissions, yet the separation of charge carriers integrative regulation oxidation activation sites remain challenging. Here, BiVO4 /g-C3 N4 (BVO/CN) as such prototype is constructed spatially separated dual CoOx clusters imidazolium ionic liquids (IL) toward photoreduction. The optimized -BVO/CN-IL delivers ≈80-fold CO production rate without H2 evolution compared urea-C3 counterpart, together nearly stoichiometric O2 produced. Experimental results DFT calculations unveil cascade transfer subsequently prominent redox co-catalysis IL for holes-H2 O electrons-CO2 reduction, respectively. Moreover, in situ µs-transient absorption spectra clearly show function each cocatalyst quantitatively reveal that resulting reaches up electron efficiency 36.4% far beyond those BVO/CN (4.0%) urea-CN (0.8%), underlining exceptional synergy reaction engineering. This work provides deep insights guidelines rational design highly efficient heterojunctions precise catalytic solar fuel production.

Language: Английский

Citations

57
The Precision Defect Engineering with Nonmetallic Element Refilling Strategy in g‐C3N4 for Enhanced Photocatalytic Hydrogen Production DOI
Yujie Liu, Muhammad Tayyab,

Wenkai Pei

et al.

Small, Journal Year: 2023, Volume and Issue: 19(21)

Published: Feb. 25, 2023

Traditional defect engineering and doping strategies are considered effective means for improving H2 evolution, but the uncontrollability of modification process does not always lead to efficient activity. A defect-induced heteroatom refilling strategy is used here synthesize heteroatoms introduced carbon nitride by precisely controlling "introduction" sites on N1 sites. Density functional theory calculations show that B, P, S have stronger O adsorption dissociation capacity than traditional doping, which makes it an optimal production path. The large internal electric field strength heteroatom-refilled catalysts leads fast electron transfer hydrogen best sample up 20.9 mmol g-1 h-1 . This work provides a reliable clear insight into controlled photocatalysts universal typical co-catalyst systems production.

Language: Английский

Citations

47
Ultrathin Defective Nanosheet Subunit ZnIn2S4 Hollow Nanoflowers for Efficient Photocatalytic Hydrogen Evolution DOI Creative Commons
Shuoping Ding, Igor Medić, Norbert Steinfeldt

et al.

Small Structures, Journal Year: 2023, Volume and Issue: 4(10)

Published: May 18, 2023

Constructing hierarchical and ultrathin‐structured metal sulfides is beneficial for achieving high‐efficiency hydrogen evolution catalysts. Herein, ZnIn 2 S 4 (ZIS) hollow nanoflowers (HNFs) composed of ultrathin nanosheets are creatively synthesized via a facile trisodium citrate‐mediated stirring‐assisted solvothermal method. Experimental results reveal that the synergy effect ethanol, citrate, continuous stirring during synthesis process play significant role in optimizing microstructure as well physicochemical properties as‐prepared ZIS samples. Importantly, fabricated HNFs with thinnest (2.28 nm) manifest highest average photocatalytic generation rate 301.5 μmol h −1 , which 2.3 times higher than pristine microspheres nanoparticles Pt cocatalyst triethanolamine (TEOA) sacrificial agent outperforms most reported ZnIn2S4‐based materials under similar testing conditions. Moreover, optimized sample also shows 0.53 −1. pure water without any cocatalyst. This controllable agitation reaction mixture hydro/solvothermal offers an eco‐friendly scalable approach tuning nanomaterials enhanced performance various applications.

Language: Английский

Citations

45
Unveiling pH‐Dependent Adsorption Strength of *CO2− Intermediate over High‐Density Sn Single Atom Catalyst for Acidic CO2‐to‐HCOOH Electroreduction DOI Creative Commons
Bin Sun,

Zaiqi Li,

Difei Xiao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(14)

Published: Feb. 16, 2024

Abstract The acidic electrochemical CO 2 reduction reaction (CO RR) for direct formic acid (HCOOH) production holds promise in meeting the carbon‐neutral target, yet its performance is hindered by competing hydrogen evolution (HER). Understanding adsorption strength of key intermediates electrolyte indispensable to favor RR over HER. In this work, high‐density Sn single atom catalysts (SACs) were prepared and used as catalyst, reveal pH‐dependent coverage *CO − intermediatethat enables enhanced towards HCOOH production. At pH=3, SACs could deliver a high Faradaic efficiency (90.8 %) formation corresponding partial current density up −178.5 mA cm −2 . detailed situ attenuated total reflection Fourier transform infrared (ATR‐FTIR) spectroscopic studies that favorable alkaline microenvironment formed near surface SACs, even electrolyte. More importantly, intermediate unravelled which turn affects competition between HER

Language: Английский

Citations

35
Surface Engineered Single‐atom Systems for Energy Conversion DOI

Yutang Yu,

Zijian Zhu, Hongwei Huang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

Language: Английский

Citations

29
Challenges and opportunities of atomic-scales reactive sites in thriving electrochemical CO2 reduction reaction DOI
Pengliang Sun, Sailin Liu, Xiong Zheng

et al.

Nano Today, Journal Year: 2024, Volume and Issue: 55, P. 102152 - 102152

Published: Jan. 13, 2024

Language: Английский

Citations

24
Reactive capture and electrochemical conversion of CO2 with ionic liquids and deep eutectic solvents DOI Creative Commons
Saudagar Dongare, Muhammad Zeeshan,

Ahmet Safa Aydogdu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(17), P. 8563 - 8631

Published: Jan. 1, 2024

Ionic liquids (ILs) and deep eutectic solvents (DESs) have tremendous potential for reactive capture of CO 2 , due to their highly properties, including a wide electrochemical stability window, low volatility, high solubility.

Language: Английский

Citations

21