Compressive Strain Modulation of Single Iron Sites on Helical Carbon Support Boosts Electrocatalytic Oxygen Reduction DOI
Jia Yang, Zhiyuan Wang, Chunxiang Huang

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(42), P. 22722 - 22728

Published: Aug. 17, 2021

Abstract Designing and modulating the local structure of metal sites is key to gain unique selectivity high activity single site catalysts. Herein, we report strain engineering curved atomic iron‐nitrogen boost electrocatalytic activity. First, a helical carbon with abundant high‐curvature surface realized by carbonization polypyrrole that templated from self‐assembled chiral surfactants. The introduces compressive on supported Fe−N 4 sites. Consequently, 1.5 % compressed bonds exhibit downshifted d‐band center than planar Such change can weaken bonding strength between oxygenated intermediates sites, resulting much smaller energy barrier for oxygen reduction. Catalytic tests further demonstrate kinetic current density 7.922 mA cm −2 at 0.9 V vs. RHE obtained in alkaline media which 31 times higher ones. Our findings shed light three‐dimensional boosting catalytic via engineering.

Language: Английский

Single-atom catalysis in advanced oxidation processes for environmental remediation DOI

Yanan Shang,

Xing Xu,

Baoyu Gao

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 5281 - 5322

Published: Jan. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Language: Английский

Citations

754

Polymer-Derived Heteroatom-Doped Porous Carbon Materials DOI
Hong Wang, Yue Shao,

Shilin Mei

et al.

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(17), P. 9363 - 9419

Published: Aug. 6, 2020

Heteroatom-doped porous carbon materials (HPCMs) have found extensive applications in adsorption/separation, organic catalysis, sensing, and energy conversion/storage. The judicious choice of precursors is crucial for the manufacture HPCMs with specific usages maximization their functions. In this regard, polymers as demonstrated great promise because versatile molecular nanoscale structures, modulatable chemical composition, rich processing techniques to generate textures that, combination proper solid-state chemistry, can be maintained throughout carbonization. This Review comprehensively surveys progress polymer-derived functional terms how produce control porosities, heteroatom doping effects, morphologies related use. First, we summarize discuss synthetic approaches, including hard soft templating methods well direct synthesis strategies employing pores and/or heteroatoms HPCMs. Second, effects on thermal stability, electronic optical properties, surface chemistry Specifically, effect, which involves both single-type codoping two or more types into network, discussed. Considering significance application spectrum, potential choices suitable polymeric precisely regulate are presented. Finally, provide our perspective predefine structures by using realize current fields generation/conversion environmental remediation. We believe that these analyses deductions valuable a systematic understanding will serve source inspiration design future

Language: Английский

Citations

674

Intrinsic Electrocatalytic Activity Regulation of M–N–C Single‐Atom Catalysts for the Oxygen Reduction Reaction DOI
Zhao Chang-xin, Bo‐Quan Li, Jia‐Ning Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(9), P. 4448 - 4463

Published: April 21, 2020

Abstract Single‐atom catalysts (SACs) with highly active sites atomically dispersed on substrates exhibit unique advantages regarding maximum atomic efficiency, abundant chemical structures, and extraordinary catalytic performances for multiple important reactions. In particular, M–N–C SACs (M=transition metal atom) demonstrate optimal electrocatalytic activity the oxygen reduction reaction (ORR) have attracted extensive attention recently. Despite substantial efforts in fabricating various SACs, principles regulating intrinsic of their not been sufficiently studied. this Review, we summarize regulation strategies promoting ORR by modulation center atoms, coordinated environmental guest groups. Theoretical calculations experimental investigations are both included to afford a comprehensive understanding structure–performance relationship. Finally, future directions developing advanced other analogous reactions proposed.

Language: Английский

Citations

597

Theoretical Understandings of Graphene-based Metal Single-Atom Catalysts: Stability and Catalytic Performance DOI
Hongying Zhuo, Xin Zhang, Jinxia Liang

et al.

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 12315 - 12341

Published: Oct. 28, 2020

Research on heterogeneous single-atom catalysts (SACs) has become an emerging frontier in catalysis science because of their advantages high utilization noble metals, precisely identified active sites, selectivity, and tunable activity. Graphene, as a one-atom-thick two-dimensional carbon material with unique structural electronic properties, been reported to be superb support for SACs. Herein, we provide overview recent progress investigations graphene-based Among the large number publications, will selectively focus stability metal single-atoms (SAs) anchored different sites graphene catalytic performances SACs chemical reactions, including thermocatalysis electrocatalysis. We summarize fundamental understandings structures intrinsic connection properties SACs, also brief perspective future design efficient graphene-like materials.

Language: Английский

Citations

530

General synthesis of single-atom catalysts with high metal loading using graphene quantum dots DOI
Chuan Xia, Yunrui Qiu, Xia Yang

et al.

Nature Chemistry, Journal Year: 2021, Volume and Issue: 13(9), P. 887 - 894

Published: June 24, 2021

Language: Английский

Citations

516

Engineered carbon supported single iron atom sites and iron clusters from Fe-rich Enteromorpha for Fenton-like reactions via nonradical pathways DOI

Lijng Peng,

Xiaoguang Duan,

Yanan Shang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 287, P. 119963 - 119963

Published: Feb. 7, 2021

Language: Английский

Citations

402

A Review on Challenges and Successes in Atomic-Scale Design of Catalysts for Electrochemical Synthesis of Hydrogen Peroxide DOI

Samira Siahrostami,

Santiago Jimenez-Villegas,

Amir Hassan Bagherzadeh Mostaghimi

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(14), P. 7495 - 7511

Published: June 10, 2020

Hydrogen peroxide is a valuable chemical oxidant with wide range of applications in variety industrial processes, especially water sanitization. Electrochemical synthesis hydrogen (H2O2) through two-electron oxygen reduction reaction (2e-ORR) or oxidation (2e-WOR) has emerged as an appealing process for onsite production this chemically oxidant. On-site produced H2O2 can be applied wastewater treatment remote locations any where needed oxidizing agent. This Review studies the theoretical efforts understanding challenges catalysis electrochemical well providing design principles more efficient catalyst materials.

Language: Английский

Citations

382

Electrocatalysis of Single-Atom Sites: Impacts of Atomic Coordination DOI
Bingzhang Lu, Qiming Liu, Shaowei Chen

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(14), P. 7584 - 7618

Published: June 11, 2020

Single metal atoms embedded within select supporting matrices have shown great potential in the development of high-efficiency, low-cost electrocatalysts because maximal atom utilization and mass activity. As single are stabilized by coordination bonds with substrate, strong metal–support interactions can be exploited for ready manipulation electrocatalytic activity selectivity toward target reactions. However, most single-atom catalysts (SACs) prepared pyrolysis contain a wide range structures. Resolving atomic configurations moieties represents critical first step establishment an unambiguous correlation between SAC structure In this Review, we summarize recent progress studies electrocatalysts, focus on impacts sites activities series reactions that important various electrochemical energy technologies, such as hydrogen evolution reaction, oxygen reduction nitrogen CO2 so on. The survey entails SACs, from noble metals (e.g., Pt, Pd, Ru, Ir, Au, etc.) to non-noble Fe, Co, Ni, Cu, etc.), supported variety substrate materials pristine doped carbon, metal, oxide, sulfide, etc.). Finally, Review concludes perspective highlighting promises challenges further SACs context chemistry.

Language: Английский

Citations

338

Lightweight Ni Foam‐Based Ultra‐Broadband Electromagnetic Wave Absorber DOI
Ming Qin, Limin Zhang, Xiaoru Zhao

et al.

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(30)

Published: May 18, 2021

Abstract Skin effect and high density are the main reasons that restrict search of lightweight high‐performance metal‐based electromagnetic (EM) wave absorbing materials. Although nanostructured metal materials have been fabricated to solve above problems, poor dispersibility chemical stability issues brought about by surface energy due existing nano‐size effect. In this work, Ni foam with NiO/NiFe 2 O 4 in situ growth composites a facile universal route as an effective alternative EM absorber. Impressively, it is found structure /Ni components can synergistically boost absorption capacity. detail, impedance matching from dissipation interfacial polarization defect induced provided mainly contributes its ultra‐broadband performance. As result, as‐prepared sample (0.06 g·cm −3 ) delivers wide bandwidth 14.24 GHz thin thickness 0.6 mm, well as, specific 19444.4 GHz·g −1 ·cm −2 . This work sheds light on novel view synergistic behaviors demonstrates new pathway for preparation absorbers.

Language: Английский

Citations

338

Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts DOI Creative Commons
Wenchao Wan, Yonggui Zhao, Shiqian Wei

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Sept. 22, 2021

Abstract Single-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support the rational design of single-site dual-site single-atom catalysts. Catalysts single Fe sites exhibit impressive oxygen reduction reaction activity half-wave 0.89 V vs. RHE. find that Ni are favorable to promote key structural reconstruction into bridging Ni-O-Fe bonds in NiFe SAC. Meanwhile, newly formed create spin channels electron transfer, resulting significant improvement evolution an overpotential 270 mV at 10 mA cm −2 . further reveal water oxidation follows pathway through deprotonation *OH both sites, leading formation O 2 atop sites.

Language: Английский

Citations

295