Constructing an Active Sulfur‐Vacancy‐Rich Surface for Selective *CH3‐CH3 Coupling in CO2‐to‐C2H6 Conversion With 92% Selectivity DOI Open Access

Xiaonan Yang,

Liteng Ren,

Zhiheng Chen

et al.

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

Published: Nov. 6, 2024

Abstract To achieve high selectivity in photocatalytic CO 2 reduction to C 2+ products, increasing the number of adsorption sites and lowering energy barriers for key intermediates are critical. A ZnIn S 4 (ZIS)/MoO 3‐x (Z‐M) photocatalyst is presented, which plasmonic MoO generates hot electrons, creating a multielectron environment ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal reduces formation sulfur vacancies (S V ) ZIS, thereby enhancing activation. The ‐rich surface lowers barrier forming HCOO * −0.33 eV whereas COOH 0.77 eV. Successive hydrogenation leads CH , converts 3 with an −0.63 ‐CH 0.54 eV, lower than 0.73 form H . Thus, Z‐M preferentially produces 6 over Under visible light, achieves ‐to‐C conversion rate 467.3 µmol g −1 h 92.0% selectivity. This work highlights dual role photocatalysts improving production reduction.

Language: Английский

Stability Issues in Electrochemical CO2 Reduction: Recent Advances in Fundamental Understanding and Design Strategies DOI Open Access
Wenchuan Lai, Yan Qiao, Yanan Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: Aug. 11, 2023

Electrochemical CO2 reduction reaction (CO2 RR) offers a promising approach to close the anthropogenic carbon cycle and store intermittent renewable energy in fuels or chemicals. On path commercializing this technology, achieving long-term operation stability is central requirement but still confronts challenges. This motivates organize present review systematically discuss issue of RR. starts from fundamental understanding on destabilization mechanisms RR, with focus degradation electrocatalyst change microenvironment during continuous electrolysis. Subsequently, recent efforts catalyst design stabilize active sites are summarized, where increasing atomic binding strength resist surface reconstruction highlighted. Next, optimization electrolysis system enhance by maintaining especially mitigating flooding carbonate problems demonstrated. The manipulation conditions also enables prolong RR lifespan through recovering catalytically mass transport process. finally ends up indicating challenges future opportunities.

Language: Английский

Citations

88
A Guideline to Determine Faradaic Efficiency in Electrochemical CO2 Reduction DOI Open Access
N. C. Dutta, Debabrata Bagchi,

Geetansh Chawla

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(1), P. 323 - 328

Published: Jan. 2, 2024

ADVERTISEMENT RETURN TO ISSUEPREVViewpointNEXTA Guideline to Determine Faradaic Efficiency in Electrochemical CO2 ReductionNilutpal DuttaNilutpal DuttaNew Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore 560064, IndiaSchool of Materials (SAMat), IndiaMore by Nilutpal Duttahttps://orcid.org/0009-0005-4237-5518, Debabrata BagchiDebabrata BagchiNew Bagchihttps://orcid.org/0000-0001-9922-2073, Geetansh ChawlaGeetansh ChawlaNew Chawla, and Sebastian C. Peter*Sebastian PeterNew India*Phone: 080-22082998. Email: [email protected], protected]More Peterhttps://orcid.org/0000-0002-5211-446XCite this: ACS Energy Lett. 2024, 9, 1, 323–328Publication Date (Web):January 2, 2024Publication History Received4 November 2023Accepted7 December 2023Published online2 January 2024Published inissue 12 2024https://pubs.acs.org/doi/10.1021/acsenergylett.3c02362https://doi.org/10.1021/acsenergylett.3c02362article-commentaryACS PublicationsCopyright © 2024 American Chemical Society. This publication is available under these Terms Use. Request reuse permissions free access through this site. Learn MoreArticle Views10691Altmetric-Citations3LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum full text article downloads since 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail (3 MB) Get e-AlertscloseSupporting Info (1)»Supporting Information Supporting SUBJECTS:Calibration,Catalysts,Chemical calculations,Electrical properties,Liquids e-Alerts

Language: Английский

Citations

27
Engineered Two-Dimensional Transition Metal Dichalcogenides for Energy Conversion and Storage DOI
Soumyabrata Roy, Antony Joseph, Xiang Zhang

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(16), P. 9376 - 9456

Published: July 23, 2024

Designing efficient and cost-effective materials is pivotal to solving the key scientific technological challenges at interface of energy, environment, sustainability for achieving NetZero. Two-dimensional transition metal dichalcogenides (2D TMDs) represent a unique class that have catered myriad energy conversion storage (ECS) applications. Their uniqueness arises from their ultra-thin nature, high fractions atoms residing on surfaces, rich chemical compositions featuring diverse metals chalcogens, remarkable tunability across multiple length scales. Specifically, electronic/electrical, optical, thermal properties 2D TMDs been widely exploited electrochemical (e.g., electrocatalytic water splitting), anodes in alkali ion batteries supercapacitors), photocatalysis, photovoltaic devices, thermoelectric Furthermore, performances can be greatly boosted by judicious structural tuning through phase, size, composition, defect, dopant, topological, heterostructure engineering. The challenge, however, design control such engineering levers, optimally specifically, maximize performance outcomes targeted In this review we discuss, highlight, provide insights significant advancements ongoing research directions approaches improving potential ECS

Language: Английский

Citations

27
Deriving multi-metal nanomaterials on metal–organic framework platforms for oxygen electrocatalysis DOI
Mingjin Cui, Bo Xu, Yu Ding

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(12), P. 4010 - 4035

Published: Jan. 1, 2024

Synthetic strategies and oxygen electrocatalytic applications of high-entropy alloy multi-metal nanomaterials derived on metal–organic frameworks.

Language: Английский

Citations

26
Catalyst design for electrochemical CO2 reduction to ethylene DOI Creative Commons
Yuanjun Chen, Rui Kai Miao, Christine J. Yu

et al.

Matter, Journal Year: 2024, Volume and Issue: 7(1), P. 25 - 37

Published: Jan. 1, 2024

Language: Английский

Citations

24
Tailoring Activation Intermediates of CO2 Initiates C–N Coupling for Highly Selective Urea Electrosynthesis DOI
Chao Zhao, Jin Yu, Jing Yuan

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Electrocatalyzed reduction of CO2 and NO3- to synthesize urea is a highly desirable, but challenging reaction. The bottleneck this reaction the C-N coupling intermediates. In particular, uncertainty multielectron intermediates severely affects selectivity activity processes involving multiple electron proton transfers. Here, we present novel tandem catalyst with two compatible single-atom active sites Au Cu on red phosphorus (RP-AuCu) that efficiently converts urea. Experimental theoretical prediction results confirmed center promotes transfer between molecules phosphorus, thereby regulating activation produce electrophilic *COOH. addition, can enhance attack *COOH species *NH2, thus promoting selective formation bonds. Consequently, RP-AuCu exhibited yield 22.9 mmol gcat.-1 h-1 Faraday efficiency 88.5% (-0.6 VRHE), representing one highest levels electrocatalytic synthesis. This work deepens understanding mechanism provides an interesting design approach for efficient sustainable production compounds.

Language: Английский

Citations

2
Cooperative Copper Single‐Atom Catalyst in 2D Carbon Nitride for Enhanced CO2 Electrolysis to Methane DOI
Soumyabrata Roy, Zhengyuan Li, Zhiwen Chen

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(13)

Published: Aug. 12, 2023

Abstract Renewable‐electricity‐powered carbon dioxide (CO 2 ) reduction (eCO R) to high‐value fuels like methane (CH 4 holds the potential close cycle at meaningful scales. However, this kinetically staggered 8‐electron multistep suffers from inadequate catalytic efficiency and current density. Atomic Cu‐structures can boost eCO R‐to‐CH selectivity due enhanced intermediate binding energies (BEs) resulting favorably shifted d‐band centers. In work, 2D nitride (CN) matrices, viz. Na‐polyheptazine (PHI) Li‐polytriazine imides (PTI), are exploited host Cu–N type single‐atom sites with high density (≈1.5 at%), via a facile metal‐ion exchange process. Optimized Cu loading in nanocrystalline Cu‐PTI maximizes performance Faradaic (FE CH4 of ≈68% partial 348 mA cm −2 −0.84 V vs reversible hydrogen electrode (RHE), surpassing state‐of‐the‐art catalysts. Multi‐Cu substituted N‐appended nanopores CN frameworks yield thermodynamically stable quasi‐dual/triple large interatomic distances dictated by pore dimensions. First‐principles calculations elucidate relative Cu–CN cooperative effects between matrices how local environment dictates adsorbate BEs, states, CO ‐to‐CH energy profile landscape. The 9N pores Cu–Cu that synergistically enhance kinetics rate‐limiting steps pathway.

Language: Английский

Citations

41
Efficient Electrocatalytic Reduction of CO2 to Ethanol Enhanced by Spacing Effect of CuCu in Cu2‐xSe Nanosheets DOI
Hongzhi Wang,

Xinze Bi,

Yifan Yan

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(25)

Published: March 10, 2023

Abstract It is highly desired yet challenging to strategically steer carbon dioxide (CO 2 ) electroreduction reaction ER) toward ethanol (EtOH) with high activity, which provides a promising way for intermittent renewable energy reservation. Controlling spatial distance between the adjoining active centers and promoting CC coupling progress are crucial realize this purpose. Herein, ultrathin 2D Cu 2‐x Se prepared abundant vacancies, where CuCu around vacancies effectively shortened because of lattice stress. Besides, moderate induced by can significantly decrease Gibbs free asymmetric *CO*CHO progress, change local charge distribution, valence state atoms increase electron‐donating capacity dual sites. Combining experimental observations density functional theory simulations, sites 2.51 Å in V ‐Cu sample catalyze CO ER EtOH selectivity potential range from −0.4 −1.6 V, reach highest faradaic efficiency 68.1% at −0.8 V. This work reveals influence spacing effect on selectivity, new idea future design catalysts chain elongation reaction, bring extensive attention.

Language: Английский

Citations

35
Electricity-Driven Microbial Metabolism of Carbon and Nitrogen: A Waste-to-Resource Solution DOI
Na Chu, Yong Jiang,

Qinjun Liang

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(11), P. 4379 - 4395

Published: March 6, 2023

Electricity-driven microbial metabolism relies on the extracellular electron transfer (EET) process between microbes and electrodes provides promise for resource recovery from wastewater industrial discharges. Over past decades, tremendous efforts have been dedicated to designing electrocatalysts microbes, as well hybrid systems push this approach toward adoption. This paper summarizes these advances in order facilitate a better understanding of electricity-driven sustainable waste-to-resource solution. Quantitative comparisons electrosynthesis abiotic are made, strategy electrocatalyst-assisted is critically discussed. Nitrogen processes including electrochemical N2 fixation, electrocatalytic reduction, dissimilatory nitrate reduction ammonium (DNRA), ammonia (Abio-NRA) systematically reviewed. Furthermore, synchronous carbon nitrogen using inorganic-biological discussed, advanced physicochemical, microbial, characterizations involved field. Finally, perspectives future trends presented. The valuable insights potential contribution valorization waste green society.

Language: Английский

Citations

29
Heterojunction Engineering for Electrocatalytic Applications DOI
Santanu Kumar Pal, Tanbir Ahmed, Sakila Khatun

et al.

ACS Applied Energy Materials, Journal Year: 2023, Volume and Issue: 6(15), P. 7737 - 7784

Published: June 22, 2023

Production of green hydrogen from the electrolysis water is considered to be one most desirable processes address clean energy demand. However, a high barrier and an economically unsustainable nature limit process toward practical implementation in extensive way. The designing electrocatalyst accompanied by defect engineering, heteroatom doping, strain creation are known effective strategies make efficient. Recently, construction heterojunctions with combination materials desired band structures smart approach promoting electrocatalytic activities attaining charge redistribution manipulating electronic structure at interface. present review elaborately discusses possible heterojunctions, alterations interface, insight thermodynamics, causes for boosting activities. heterojunction-based electrocatalysts found not only oxygen evolution reactions reactions, but also very useful various electrochemical oxidation as well reduction involving small molecules undergoing decomposition low energy. Having such specialty, there no doubt that going primary choices researchers coming years.

Language: Английский

Citations

28