Double‐Tuned RuCo Dual Metal Single Atoms and Nanoalloy with Synchronously Expedited Volmer/Tafel Kinetics for Effective and Ultrastable Ampere‐Level Current Density Hydrogen Production

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(40)

Published: July 31, 2023

Abstract Alkaline water electrolysis system is of general interest but impeded by the unsatisfactory hydrogen evolution reaction (HER) performance under ampere‐level current density. Herein, synchronous modification complicated Volmer/Tafel kinetics effectuated for attaining density production via engineering double‐tuned RuCo nanoalloy and dual metal single atoms on hierarchical N‐doped mesoporous carbon (RuCo@Ru SA Co ‐NMC). The electronic structure Ru sites in can be synergistically tailored adjacent atomic nanoalloy, which makes it achieve faster Volmer with rapid adsorption/dissociation transfer rates toward adsorbed hydroxyl. While alloyed undertake optimized Tafel boosted hydrogen. Accordingly, RuCo@Ru ‐NMC exhibits ultralow HER overpotential 255 mV at 1 A cm −2 robust stability over 24 days, ultrahigh mass activity 37.2 mg −1 , turnover frequency 19.5 s . More importantly, make possess low power consumption 5.34 kWh per Nm 3 H2 estimated costs 1.197 $ kg concept emphasized this study provides guidance rational design cost‐effective catalysts production.

Language: Английский

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Advances in electrolyzer design and development for electrochemical CO₂ reduction

EcoMat, Journal Year: 2023, Volume and Issue: 5(7)

Published: April 27, 2023

Abstract In view of global energy transition and environmental issues, electrochemical conversion carbon dioxide (CO 2 ) to high value‐added chemicals by using clean renewable electricity, as an advanced capture, utilization storage (CCUS) technology, demonstrates a promising approach reach the neutrality with additional economic benefits well. Over past decade, various new valid catalysts in CO reduction (ECO2R) have been designed intensively investigated. Unfortunately, constructing appropriate ECO2R electrolyzer rate long‐term stability unleash full potential electrocatalysts remains recognized challenge, especially it has not yet attracted attention. This review summarizes progress reactor their corresponding structure characteristics/ performance. Besides, current challenges bottlenecks CO2RR are discussed. We aim introduce advances detail offer enlightenment for large‐scale industrial application ECO2R. image

Language: Английский

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Isolated Tin(IV) Active Sites for Highly Efficient Electroreduction of CO₂ to CH₄ in Neutral Aqueous Solution

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(22)

Published: Feb. 24, 2023

The development of efficient electrocatalysts with non-copper metal sites for electrochemical CO2 reduction reactions (eCO2 RR) to hydrocarbons and oxygenates is highly desirable, but still a great challenge. Herein, stable metal-organic framework (DMA)4 [Sn2 (THO)2 ] (Sn-THO, THO6- = triphenylene-2,3,6,7,10,11-hexakis(olate), DMA dimethylammonium) isolated distorted octahedral SnO62- active reported as an electrocatalyst eCO2 RR, showing exceptional performance RR the CH4 product rather than common products formate CO Sn-based catalysts. partial current density reaches high value 34.5 mA cm-2 , surpassing most copper-based all non-Cu metal-based Our experimental theoretical results revealed that site favors formation key *OCOH species produce can greatly inhibit *OCHO *COOH *HCOOH *CO, respectively.

Language: Английский

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Solar driven CO₂reduction: from materials to devices

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(24), P. 12499 - 12520

Published: Jan. 1, 2023

Solar driven CO 2 reduction is a promising technology for achieving carbon neutrality. The optimized photo-absorber, catalyst and device their synergistic operation are essential realizing highly efficient solar system.

Language: Английский

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Homogeneous Vacancies-Enhanced Orbital Hybridization for Selective and Efficient CO₂-to-CO Electrocatalysis

Nano Letters, Journal Year: 2023, Volume and Issue: 23(20), P. 9227 - 9234

Published: Oct. 4, 2023

Crafting vacancies offers an efficient route to upgrade the selectivity and productivity of nanomaterials for CO2 electroreduction. However, defective nanoelectrocatalysts bear catalytically active mostly on their surface, with rest interior atoms adiaphorous CO2-to-product conversion. Herein, taking nanosilver as a prototype, we arouse catalytic ability internal by creating homogeneous realized via electrochemical reconstruction silver halides. The vacancies-rich nanosilver, compared surface vacancies-dominated counterpart, features more positive d-band center trigger intensified hybridization Ag_d orbital C_P *COOH intermediate, leading accelerated CO2-to-CO transformation. These structural electronic merits allow large-area (9 cm-2) electrode generate nearly pure CO CO/H2 Faradaic efficiency ratio 6932 at applied current 7.5 A. findings highlight potential designing new-type defects in realizing industrialization electrocatalytic reduction.

Language: Английский

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MOF‐derived 1D/3D N‐doped porous carbon for spatially confined electrochemical CO₂ reduction to adjustable syngas

Carbon Energy, Journal Year: 2024, Volume and Issue: 6(8)

Published: March 19, 2024

Abstract Electrochemical reduction of CO 2 to syngas (CO and H ) offers an efficient way mitigate carbon emissions store intermittent renewable energy in chemicals. Herein, the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous (1D/3D NPC) is prepared by carbonizing composite Zn‐MOF‐74 crystals situ grown on a commercial melamine sponge (MS), for electrochemical reaction RR). The 1D/3D NPC exhibits high CO/H ratio (5.06) yield (31 mmol g −1 h at −0.55 V, which are 13.7 times 21.4 those 1D (derived from Zn‐MOF‐74) N‐doped (carbonized MS), respectively. This attributed unique spatial environment NPC, increases adsorption capacity promotes electron transfer 3D framework carbon, improving kinetics RR. Experimental results charge density difference plots indicate that active site RR positively charged atom adjacent graphitic N HER pyridinic carbon. presence pyrrolic reduces number transfer, decreasing activity related distribution species specific surface area, determined degree confinement effect. ratios can be regulated adjusting carbonization temperature adjust Given low cost feedstock easy strategy, catalysts have great potential industrial application.

Language: Английский

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Simultaneously Engineering the First and Second Coordination Shells of Single Iron Catalysts for Enhanced Oxygen Reduction

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 10, 2024

Abstract The atomically dispersed Fe‐N 4 active site presents enormous potential for various renewable energy conversions. Despite its already remarkable catalytic performance, the local atomic microenvironment of each Fe atom can be regulated to further enhance efficiency. Herein, a novel conceptual strategy that utilizes simple salt‐template polymerization method simultaneously adjust first coordination shell (Fe‐N 3 S 1 ) and second (C–S–C, structure similar thiophene) isolated atoms is proposed. Theoretical studies suggest this approach redistribute charge density in MN moiety, lowering d‐band center metal site. This weakens binding oxygenated intermediates, enhancing oxygen reduction reaction (ORR) activity when compared only implementing regulation. Based on above discovery, single electrocatalyst with optimal ‐S moiety incorporated nitrogen, sulfur co‐doped graphene (Fe‐SAc/NSG) designed synthesized. Fe‐SAc/NSG catalyst exhibits excellent alkaline ORR activity, exceeding benchmark Pt/C most Fe‐SAc electrocatalysts, as well superior stability Zn–air battery. work aims pave way creating highly catalysts through localized regulation their structure.

Language: Английский

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Modulating d-orbital occupancy via a coupled interfacial-local electric field for electrocatalytic N2 fixation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 345, P. 123700 - 123700

Published: Jan. 4, 2024

Language: Английский

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Self‐Encapsulated Ni Nanoparticles on Delignified Wood Carbon for Efficient Urea‐Assisted Hydrogen Production

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

Published: Oct. 8, 2024

Abstract Developing efficient, low‐cost electrocatalysts for industrial‐level hydrogen production remains a significant challenge. Here lattice‐distorted Ni nanoparticles (NPs) encapsulated within nitrogen‐doped carbon shell on delignified wood (Ni‐NC@DWC) are constructed through chitosan‐induced assembly and the pyrolysis process. Experimental theoretical results indicate that lattice distortion due to strong metal‐support interactions, boosts electron transfer reaction intermediate adsorption/desorption, enhancing both urea oxidation (UOR) evolution (HER). Interestingly, active center 3+ ‐O is dynamically cyclically generated during UOR. When utilized as self‐standing electrode in an alkaline electrolyte, Ni‐NC@DWC exhibits low potentials of 24 mV 1.244 V at 100 mA cm −2 HER UOR, respectively. Moreover, achieves ultrasmall cell voltage 1.13 urea‐assisted water splitting can operate stably over 1000 h. Furthermore, when it self‐assembled anion exchange membrane (AEM) electrolyzer, requires only 1.62 2000 industrial operates 150 h without degradation, confirming highly attractive economical, sustainable, scalable production.

Language: Английский

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p‐d Orbital Hybridization in Ag‐based Electrocatalysts for Enhanced Nitrate‐to‐Ammonia Conversion

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 8, 2024

Considering the substantial role of ammonia, developing highly efficient electrocatalysts for nitrate-to-ammonia conversion has attracted increasing interest. Herein, we proposed a feasible strategy p-d orbital hybridization via doping p-block metals in an Ag host, which drastically promotes performance nitrate adsorption and disassociation. Typically, Sn-doped catalyst (SnAg) delivers maximum Faradaic efficiency (FE) 95.5±1.85 % NH

Language: Английский

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