Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO2 conversion to C1C2 products DOI Creative Commons
Sue‐Faye Ng,

Joel Jie Foo,

Wee‐Jun Ong

et al.

InfoMat, Journal Year: 2022, Volume and Issue: 4(1)

Published: Jan. 1, 2022

CO2 capture and conversion has been prospected as an auspicious technology to simultaneously tackle the rise in global emission produce value-added fuels with goal of accomplishing carbon neutrality. A sustainable route achieve this is via utilization solar energy, thereby harnessing abundant nonexhaustive resource shift our reliance away from rapidly depleting fossil fuels. Graphitic nitride (g-C3N4) its allotrope have earned rank a fascinating metal-free photocatalyst due superior stability, high surface-area-to-volume ratio, tunable surface engineering. By leveraging these properties, robust nitride-based nanostructures are engineered for photocatalytic energy-rich C1C2 product, which indispensable chemical industry. Thus, review presents latest panorama experimental computational research on tuning local electronic, coordination environment, charge dynamics optical properties low-dimensional allotropes toward highly selective efficient photoconversion. To name few, structural engineering, point-defect heterojunction construction, cocatalyst loading. advance frontier, critical insights elucidated establish structure-performance relationship unravel primary factors dictating selectivity molecules reduction. External-field assisted photocatalysis such electric (photoelectro-) heat (photothermal) discussed uncover synergistic contributions that drive development photochemistry. Last, future challenges prospects outlined potential application solar-driven conversion, along scale-up strategy economic viewpoint rational high-efficiency catalysts.

Language: Английский

Single-atom catalysts for photocatalytic energy conversion DOI Creative Commons
Zhong‐Hua Xue, Deyan Luan, Huabin Zhang

et al.

Joule, Journal Year: 2022, Volume and Issue: 6(1), P. 92 - 133

Published: Jan. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Language: Английский

Citations

384

Dual optimization approach to Mo single atom dispersed g-C3N4 photocatalyst: Morphology and defect evolution DOI
Chen Zhang, Deyu Qin, Yin Zhou

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 303, P. 120904 - 120904

Published: Nov. 7, 2021

Language: Английский

Citations

313

Single-Atom (Iron-Based) Catalysts: Synthesis and Applications DOI
Baljeet Singh, Manoj B. Gawande, Arun D. Kute

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(21), P. 13620 - 13697

Published: Oct. 13, 2021

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which heterogenized on inert supports such as graphene, porous carbon, and oxides. Their thermal stability, electronic properties, catalytic activities can be controlled via interactions between the center neighboring heteroatoms nitrogen, oxygen, sulfur. Due to atomic dispersion amount required for catalysis decreased, thus offering new possibilities control selectivity a given transformation well improve catalyst turnover frequencies numbers. This review aims comprehensively summarize synthesis Fe-SACs with focus anchoring single atoms (SA) carbon/graphene supports. The characterization these advanced materials using various spectroscopic techniques their applications in diverse research areas described. When applicable, mechanistic investigations conducted understand specific behavior Fe-SACs-based highlighted, including use theoretical models.

Language: Английский

Citations

240

Single‐atom catalysis for carbon neutrality DOI Creative Commons
Ligang Wang, Dingsheng Wang, Yadong Li

et al.

Carbon Energy, Journal Year: 2022, Volume and Issue: 4(6), P. 1021 - 1079

Published: July 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Language: Английский

Citations

206

Isolating Single and Few Atoms for Enhanced Catalysis DOI Creative Commons
Chen Yang, Jian Lin, Baohua Jia

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(39)

Published: May 17, 2022

Abstract Atomically dispersed metal catalysts have triggered great interest in the field of catalysis owing to their unique features. Isolated single or few atoms can be anchored on substrates via chemical bonding space confinement maximize atom utilization efficiency. The key challenge lies precisely regulating geometric and electronic structure active centers, thus significantly influencing catalytic properties. Although several reviews been published preparation, characterization, application single‐atom (SACs), comprehensive understanding SACs, dual‐atom (DACs), atomic clusters has never systematically summarized. Here, recent advances engineering local environments state‐of‐the‐art DACs, for enhanced performance are highlighted. Firstly, various synthesis approaches presented. Then, special attention is focused elucidation terms state coordination structure. Furthermore, a summary isolated applications thermocatalysis, electrocatalysis, photocatalysis provided. Finally, potential challenges future opportunities this emerging This review will pave way regulate microenvironment site boosting processes.

Language: Английский

Citations

169

Carbon nitride based materials: more than just a support for single-atom catalysis DOI
Guilherme F. S. R. Rocha, Marcos A. R. da Silva, Andrea Rogolino

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(15), P. 4878 - 4932

Published: Jan. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Language: Английский

Citations

152

Coordination modulation of iridium single-atom catalyst maximizing water oxidation activity DOI Creative Commons

Zhanwu Lei,

Wenbin Cai,

Yifei Rao

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Jan. 10, 2022

Abstract Single-atom catalysts (SACs) have attracted tremendous research interests in various energy-related fields because of their high activity, selectivity and 100% atom utilization. However, it is still a challenge to enhance the intrinsic specific activity SACs. Herein, we present an approach fabricate surface distribution density iridium (Ir) SAC on nickel-iron sulfide nanosheet arrays substrate (Ir 1 /NFS), which delivers water oxidation activity. The Ir /NFS catalyst offers low overpotential ~170 mV at current 10 mA cm −2 turnover frequency 9.85 s −1 300 1.0 M KOH solution. At same time, exhibits stability performance, reaching lifespan up 350 hours 100 . First-principles calculations reveal that electronic structures atoms are significantly regulated by substrate, endowing energetically favorable reaction pathway. This work represents promising strategy single-atom with durability for electrochemical splitting.

Language: Английский

Citations

146

Engineering graphitic carbon nitride (g-C3N4) for catalytic reduction of CO2to fuels and chemicals: strategy and mechanism DOI

Qingqing Lu,

Kamel Eid, Wenpeng Li

et al.

Green Chemistry, Journal Year: 2021, Volume and Issue: 23(15), P. 5394 - 5428

Published: Jan. 1, 2021

This review summarises the structural-compositional engineering of carbon nitride (g-C3N4) for electrocatalytic and photocatalytic CO2reduction to chemicals fuels experimentally theoretically.

Language: Английский

Citations

143

Recent advances of single-atom catalysts in CO2conversion DOI

Shunwu Wang,

Ligang Wang, Dingsheng Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2759 - 2803

Published: Jan. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Language: Английский

Citations

142

Synthesis and modification strategies of g-C3N4 nanosheets for photocatalytic applications DOI Creative Commons
Long Chen,

Michael A. Maigbay,

Miao Li

et al.

Advanced Powder Materials, Journal Year: 2023, Volume and Issue: 3(1), P. 100150 - 100150

Published: July 5, 2023

Graphitic carbon nitride nanosheets (CNNs) become the most promising member in family benefitted from their two-dimensional structural features. Recently, great endeavors have been made synthesis and modification of CNNs to improve photocatalytic properties, many exciting progresses gained. In order elucidate fundamentals based catalysts provide insights into rational design photocatalysis system, we describe recent progress preparation strategies applications this review. Firstly, physicochemical properties are briefly introduced. Secondly, approaches reviewed, including top-down stripping (thermal, gas, liquid, composite stripping) bottom-up precursor molecules (solvothermal, template, supramolecular self-assembly method). Subsequently, on years discussed, crystal structure design, doping, surface functionalization, constructing 2D heterojunction, anchoring single-atom. Then multifunctional g-C3N4 nanosheet materials H2 evolution, O2 overall water splitting, H2O2 production, CO2 reduction, N2 fixation, pollutant removal, organic synthesis, sensing highlighted. Finally, opportunities challenges for development high-performance systems also promising.

Language: Английский

Citations

138