Iron-based metal–organic frameworks and their derived materials for photocatalytic and photoelectrocatalytic reactions

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 499, P. 215538 - 215538

Published: Nov. 1, 2023

Language: Английский

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Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: June 14, 2024

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable efficient urea production. Herein, diatomic alloy catalyst (CuPd 1 Rh –DAA), with mutually isolated Pd atoms alloyed on Cu substrate, is theoretically designed experimentally confirmed to be highly active selective UENC catalyst. Combining theoretical computations operando spectroscopic characterizations reveals the synergistic effect –Cu sites promote via tandem catalysis mechanism, where site triggers early C–N coupling promotes *CO –to–*CO NH steps, while facilitates subsequent protonation step *COOHNH toward formation. Impressively, CuPd –DAA assembled in flow cell presents highest Faradaic efficiency 72.1% yield rate 53.2 mmol h −1 g cat at −0.5 V versus RHE, representing nearly performance among all reported catalysts.

Language: Английский

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Carbon‐Anchored Molybdenum Oxide Nanoclusters as Efficient Catalysts for the Electrosynthesis of Ammonia and Urea

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)

Published: March 13, 2023

Abstract The electrochemical NO 3 − reduction and its coupling with CO 2 can provide novel clean routes to synthesize NH urea, respectively. However, their practical application is still impeded by the lack of efficient catalysts desirable Faradaic efficiency (FE) yield rate. Herein, we report synthesis molybdenum oxide nanoclusters anchored on carbon black (MoO x /C) as electrocatalyst. It affords an outstanding FE 98.14 % rate 91.63 mg h −1 cat. in reduction. Besides, highest 27.7 a maximum urea 1431.5 μg toward also achieved. formation electron‐rich MoO highly unsaturated metal sites /C heterostructure beneficial for enhanced catalytic performance. Studies mechanism reveal that stabilization *NO *CO NOOH intermediates are critical synthesis,

Language: Английский

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Pulsed co-electrolysis of carbon dioxide and nitrate for sustainable urea synthesis

Nature Sustainability, Journal Year: 2024, Volume and Issue: 7(4), P. 442 - 451

Published: Feb. 26, 2024

Language: Английский

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Electrosynthesis of α‐Amino Acids from NO and other NO_x species over CoFe alloy‐decorated Self‐standing Carbon Fiber Membranes

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 31, 2023

Abstract The conversion of industrial exhaust gases nitrogen oxides into high‐value products is significantly meaningful for global environment and human health. And green synthesis amino acids vital biomedical research sustainable development mankind. Herein, we demonstrate an innovative approach converting nitric oxide (NO) to a series α‐amino (over 13 kinds) through electrosynthesis with α‐keto over self‐standing carbon fiber membrane CoFe alloy. essential leucine exhibits high yield 115.4 μmol h −1 corresponding Faradaic efficiency 32.4 %, gram can be obtained within 24 hours in lab as well ultra‐long stability (>240 h) the catalyst, which could convert NO NH 2 OH rapidly attacking acid subsequent hydrogenation form acid. In addition, this method also suitable other sources including gaseous or liquidus 3 − . Therefore, work not only presents promising prospects from gas nitrate‐laden waste water products, but has significant implications synthetizing catalytic science.

Language: Английский

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Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO₂ and biomass as carbon sources

SusMat, Journal Year: 2023, Volume and Issue: 3(6), P. 781 - 820

Published: Dec. 1, 2023

Abstract Thermochemical conversion of fossil resources into fuels, chemicals, and materials has rapidly increased atmospheric CO 2 levels, hindering global efforts toward achieving carbon neutrality. With the increasing push for sustainability, utilizing electrochemical technology to transform or biomass value‐added chemicals close cycle with sustainable energy sources represents a promising strategy. Expanding scope electrosynthesis is prerequisite electrification chemical manufacturing. To this end, constructing C─N bond considered priority. However, systematic review electrocatalytic processes building bonds using as not available. Accordingly, highlights research progress in organic nitrogen compounds from by coupling reactions view catalytic materials, focusing on enlightenment traditional catalysis understanding basis coupling. The possibility electrocatalysis also examined standpoints activation substrates, site, mechanism, inhibition hydrogen evolution reaction (HER). Finally, challenges prospects improved efficiency selectivity future development are discussed.

Language: Английский

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Fabrication of Nd2S3 based rGO nanohybrid via hydrothermal route and evaluation of capacitive features toward supercapacitor application

Materials Science and Engineering B, Journal Year: 2024, Volume and Issue: 301, P. 117207 - 117207

Published: Jan. 23, 2024

Language: Английский

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Electrocatalytic synthesis of C–N coupling compounds from CO₂ and nitrogenous species

SusMat, Journal Year: 2024, Volume and Issue: 4(2)

Published: March 12, 2024

Abstract The electrocatalytic synthesis of C–N coupling compounds from CO 2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality reduce environmental pollution, but also establishes a route synthesize valuable chemicals, such as urea, amide, amine. This innovative approach expands the application range product categories beyond simple carbonaceous in reduction, which is becoming rapidly advancing field. review summarizes research progress urea synthesis, using N , NO − 3 species, explores emerging trends electrosynthesis amide amine nitrogen species. Additionally, future opportunities this field are highlighted, including amino acids other containing bonds, anodic reactions water oxidation, catalytic mechanism corresponding reactions. critical captures insights aimed at accelerating development electrochemical reactions, confirming superiority method over traditional techniques.

Language: Английский

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NH₃ Electrosynthesis from N₂ Molecules: Progresses, Challenges, and Future Perspectives

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6409 - 6421

Published: Feb. 27, 2024

Green ammonia (NH3), made by using renewable electricity to split nearly limitless nitrogen (N2) molecules, is a vital platform molecule and an ideal fuel drive the sustainable development of human society without carbon dioxide emission. The NH3 electrosynthesis field currently faces dilemma low yield rate efficiency; however, decoupling overlapping issues this area providing guidelines for its directions are not trivial because it involves complex reaction process multidisciplinary entries (for example, electrochemistry, catalysis, interfaces, processes, etc.). In Perspective, we introduce classification scheme based on process, namely, direct (N2 reduction reaction) indirect (Li-mediated/plasma-enabled electrosynthesis). This categorization allows us finely decouple complicated pathways identify specific rate-determining steps/bottleneck each synthesis approach such as N2 activation, H2 evolution side reaction, solid-electrolyte interphase engineering, plasma etc. We then present detailed overview latest progresses solving these core in terms whole electrochemical system covering electrocatalysts, electrodes, electrolytes, electrolyzers, Finally, discuss research focuses promising strategies future with multiscale perspective atomistic mechanisms, nanoscale microscale electrodes/interfaces, macroscale electrolyzers/processes. It expected that Perspective will provide readers in-depth understanding bottleneck insightful guidance designing efficient systems.

Language: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

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