Alloying of Cu with Ru Enabling the Relay Catalysis for Reduction of Nitrate to Ammonia

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(19)

Published: March 5, 2023

Involving eight electron transfer process and multiple intermediates of nitrate (NO3- ) reduction reaction leads to a sluggish kinetic low Faradaic efficiency, therefore, it is essential get an insight into the mechanism develop highly efficient electrocatalyst. Herein, series reduced-graphene-oxide-supported RuCu alloy catalysts (Rux Cux /rGO) are fabricated used for direct NO3- NH3 . It found that Ru1 Cu10 /rGO shows ammonia formation rate 0.38 mmol cm-2 h-1 (loading 1 mg efficiency 98% under ultralow potential -0.05 V versus Reversible Hydrogen Electode (RHE), which comparable Ru catalyst. The activity can be attributed synergetic effect between Cu sites via relay catalysis, in exclusively NO2- exhibits superior In addition, doping tunes d-band center effectively modulates adsorption energy , promotes This electrocatalysis strategy opens new avenue developing multifunctional catalysts.

Language: Английский

---

Facilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 16, 2024

Abstract Exploring an active and cost-effective electrocatalyst alternative to carbon-supported platinum nanoparticles for alkaline hydrogen evolution reaction (HER) have remained elusive date. Here, we report a catalyst based on single atoms (SAs) doped into the hetero-interfaced Ru/RuO 2 support (referred as Pt-Ru/RuO ), which features low HER overpotential, excellent stability distinctly enhanced cost-based activity compared commercial Pt/C Ru/C in 1 M KOH. Advanced physico-chemical characterizations disclose that sluggish water dissociation is accelerated by RuO while Pt SAs metallic Ru facilitate subsequent H* combination. Theoretical calculations correlate with experimental findings. Furthermore, only requires 1.90 V reach A cm −2 delivers high price anion exchange membrane electrolyzer, outperforming benchmark Pt/C. This research offers feasible guidance developing noble metal-based catalysts performance cost toward practical H production.

Language: Английский

---

Facet Engineering of a Metal–Organic Framework Support Modulates the Microenvironment of Palladium Nanoparticles for Selective Hydrogenation

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(47)

Published: Sept. 27, 2022

The exposed facets of supported catalysts play a crucial role in catalysis; however, they are usually ignored and related studies remain rare. Herein, we have fabricated series sandwich-structured metal-organic framework composites, denoted ZIF-8X @Pd@ZIF-8 (x represents the morphology ZIF-8 core, i.e., ZIF-8C exposing (100) facet, ZIF-8RD (110) ZIF-8TRD mixed facets), featuring Pd nanoparticles deposited on specific crystal for hydrogenation p-chloronitrobenzene. electronic state is tailored by where more electron-deficient found than that @Pd@ZIF-8, leading to discriminative adsorption -NO2 -Cl groups Consequently, exhibits excellent activity (97.6 %) selectivity (98.1 p-chloroaniline. This work highlights facet engineering supports modulate microenvironment metal nanoparticles, offering promising avenue enhanced catalysis.

Language: Английский

---

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(3)

Published: Sept. 15, 2022

Abstract Single‐atom catalysts (SACs) attract extensive attention in the field of heterogeneous catalysis recent years due to maximum atom utilization and unique physical chemical properties. The gas sensing is actually a process but SACs are new this area. Although show huge potential sensing, area currently still at infancy stage. This work critically reviews advances current status single‐atom materials. General synthesis routes, characterization methods, performance indexes introduced. At end, challenges future prospects on presented from authors’ perspectives. anticipated provide insights guideline for community.

Language: Английский

---

Unconventional Bilateral Compressive Strained Ni–Ir Interface Synergistically Accelerates Alkaline Hydrogen Oxidation

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(25), P. 13805 - 13815

Published: June 15, 2023

The alkaline hydrogen oxidation reaction (HOR) involves the coupling of adsorbed (Had) and hydroxyl (OHad) species is thus orders magnitude slower than that in acid media. According to Sabatier principle, developing electrocatalysts with appropriate binding energy for both intermediates vital accelerating HOR though it still challenging. Herein, we propose an unconventional bilateral compressive strained Ni-Ir interface (Ni-Ir(BCS)) as efficient synergistic sites. Density functional theory (DFT) simulations reveal strain effect leads adsorption Had OHad, enabling their thermodynamically spontaneous kinetically preferential. Such Ni-Ir(BCS) experimentally achieved by embedding sub-nanometer Ir clusters graphene-loaded high-density Ni nanocrystals (Ni-Ir(BCS)/G). As predicted, exhibits a mass activity 7.95 2.88 times those commercial Ir/C Pt/C together much enhanced CO tolerance, respectively, ranking among most active state-of-the-art catalysts. These results provide new insights into rational design advanced involving coordinated activation multiple reactants.

Language: Английский

---

Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 14, 2023

Organic electrocatalytic conversion is an essential pathway for the green of low-cost organic compounds to high-value chemicals, which urgently demands development efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on foam cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In coupled system, Cusingle-atom-Rh requires only low voltages 1.18 V reach current densities 100 mA cm-2 generating aniline formate, with up ~100% conversion/ selectivity over ~90% formate Faraday efficiency, achieving synthesis chemicals. Density functional theory calculations reveal electron effect between host catalytic mechanism. The synergistic H*-spillover can improve process reduce energy barrier process, thus enhancing activity target product selectivity.

Language: Английский

---

Boosting Electrochemical Kinetics of NiCo₂ via MoO₂ Modification for Biomass Upgrading Assisted Hydrogen Evolution

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(20), P. 13257 - 13266

Published: Sept. 29, 2023

Converting renewable biomass into value-added chemicals is a promising strategy to reduce the dependence on fossil fuels. The development of efficient, stable, and cost-effective nonprecious metal catalytic materials significant for upgrading. Herein, 5-hydroxymethylfurfural (HMF) dehydrogenation kinetics NiCo2 nanowire tuned by MoO2 HMF electrooxidation (HMFOR)-assisted H2 evolution (HER). introduction could accelerate electron/proton transfer during HMFOR optimize adsorption behavior HMFOR/HER intermediates, which would also lower energy barrier 5-hydroxymethyl-2-furanoic acid 5-formyl-2-furancarboxylic weakening C–H/O–H bond. Consequently, NiCo2@MoO2/NF exhibits improved activity (E±10 = 1.20 VRHE/–31 mVRHE), (kNiCo2@MoO2/NF/kNiCo2/NF 2.57), 2,5-furandicarboxylic selectivity (99.2%). When coupled as two-electrode system, it requires only 1.25 V achieve 10 mA cm–2 HMFOR-assisted production. This work provides design advanced catalysts upgrading assisted

Language: Английский

---

Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Oct. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Language: Английский

---

Recent advances of single-atom alloy catalyst: Properties, synthetic methods and electrocatalytic applications

Materials Today Catalysis, Journal Year: 2023, Volume and Issue: 2, P. 100009 - 100009

Published: June 27, 2023

Developing high-performance and cost-effective electrocatalysts for clean renewable energy conversion process has been proved a promising approach to deal with the global environment issues. Single-atom alloy (SAA) catalyst, foreign metal atoms atomically dispersed in surface of host metal, combines merits conventional alloys single-atom catalysts. The maximum atomic utilization active unique structural electrical properties SAA offer great potential boosting electrocatalytic activity reducing cost manufacture. Meanwhile, well-defined sites raise an opportunity shed light on structure-activity relationship further direct synthesis high-efficiency electrocatalysts. Herein, we focus recent developments advanced catalysts discussed general SAAs. Then design principle synthetic methods were summarized. Next, highlighted practical applications SAAs chemicals production, including hydrogen evolution reaction, oxygen CO2 reduction N2 reaction other representative reactions. Finally, challenges future directions are presented.

Language: Английский

---

Manipulation of Electron Spins with Oxygen Vacancy on Amorphous/Crystalline Composite-Type Catalyst

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 1214 - 1225

Published: Dec. 27, 2023

By substituting the oxygen evolution reaction (OER) with anodic urea oxidation (UOR), it not only reduces energy consumption for green hydrogen generation but also allows purification of urea-rich wastewater. Spin engineering d orbital and oxygen-containing adsorbates has been recognized as an effective pathway enhancing performance electrocatalysts. In this work, we report fabrication a bifunctional electrocatalyst composed amorphous RuO2-coated NiO ultrathin nanosheets (a-RuO2/NiO) abundant amorphous/crystalline interfaces (HER) UOR. Impressively, 1.372 V voltage is required to attain current density 10 mA cm–2 over electrolyzer. The increased vacancies in a-RuO2/NiO by incorporation RuO2 enhance total magnetization entail numerous spin-polarized electrons during reaction, which speeds up UOR kinetics. functional theory study reveals that promote charge-carrier transfer, tailored d-band center endows optimized adsorption oxygen-generated intermediates. This kind vacancy induced toward boosting HER kinetics provides reliable reference exploration advanced

Language: Английский

---