Pd/NiMoO4/NF electrocatalysts for the efficient and ultra-stable synthesis and electrolyte-assisted extraction of glycolate

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

Published: April 4, 2024

Abstract Electrocatalytic conversion of organic small molecules is a promising technique for value-added chemical productions but suffers from high precious metal consumption, poor stability electrocatalysts and tedious product separation. Here, Pd/NiMoO 4 /NF electrocatalyst with much lowered Pd loading amount (3.5 wt.%) has been developed efficient, economic, ultra-stable glycolate synthesis, which shows Faradaic efficiency (98.9%), yield (98.8%), ultrahigh (1500 h) towards electrocatalytic ethylene glycol oxidation. Moreover, the obtained glycolic acid converted to sodium by in-situ acid-base reaction in NaOH electrolyte, atomic efficient needs no additional addition weak adsorption on catalyst surface plays significant role avoiding excessive oxidation achieving selectivity. This work may provide instructions design as well separation conversions alcohols.

Language: Английский

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Boosting electrochemical oxygen reduction to hydrogen peroxide coupled with organic oxidation

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

Published: July 19, 2024

Abstract The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O ) is appealing due its sustainability. However, efficiency compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. exhibits excellent 2e performance under alkaline conditions and achieves H yield rates of 0.73 mol g cat −1 h in H-cell 5.48 flow cell, outperforming most reported catalysts. experimental results show that atoms selectively adsorb , while nanosheets generate reactive species, synergistically enhancing production. Furthermore, coupling system integrating ethylene glycol oxidation significantly enhances rate 7.30 producing valuable glycolic acid. Moreover, convert electrolyte containing directly into downstream product sodium perborate reduce separation cost further. Techno-economic analysis validates economic viability system.

Language: Английский

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Construction of an Internal Charge Field: CoS_1.097/Ni₃S₂ Heterojunction Promotes Efficient Urea Oxidation Reaction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(38)

Published: May 6, 2024

Abstract Urea oxidation reaction (UOR) features a lower overpotential compared to the oxygen evolution (OER) during electrolysis, facilitating hydrogen (HER) at cathode. The distribution of charge plays pivotal role in promoting adsorption and cleavage chemical groups urea molecules, which can be modulated by introducing heterostructure. Herein, CoS 1.097 /Ni 3 S 2 heterojunction grown on nickel foam is designed, serving simultaneously for UOR HER. Based density functional theory (DFT) calculations, spontaneous transfer heterointerface induces formation localized electrophilic/nucleophilic regions, intelligently adsorbing electron‐donating/electron‐withdrawing activating bonds, thereby triggering decomposition. exhibits excellent catalytic activity urea, requiring only potential 1.22 V (with an 0.85 V) achieve current 100 mA cm −2 UOR, potentials 1.27 1.57 reach densities 10 , respectively, UOR//HER electrolysis cell, maintaining good stability high 60 h. Tests real urine have demonstrated performance similar that electrolyte. This work represents nearly best transition metal‐based materials applications, promising both efficient production

Language: Английский

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Pairing Electrocatalytic Reduction and Oxidation of Biomass-Derived 5-Hydroxymethylfurfural into Highly Value-Added Chemicals

JACS Au, Journal Year: 2025, Volume and Issue: 5(2), P. 937 - 947

Published: Jan. 2, 2025

Simultaneous electrocatalytic reduction and oxidation of 5-hydroxymethylfurfural (HMF) is crucial for biomass refineries. Herein, we report the unprecedentedly high efficiency nearly complete conversion biomass-derived HMF to value-added products, achieving >95% selectivity at −0.4 V vs RHE by pairing (PERO) reactions in a single electrochemical cell. At cathode, achieved 99% 2,5-dihydroxymethylfuran (DHMF) ∼99% yield under mild conditions using PtRu alloy. anode, observed HMF, perfect oxidative product 2,5-furandicarboxylic acid (FDCA), 100% Faradaic on NiCo(OOH)x nanosheets electrode. The kinetic isotope effect demonstrated that rate-controlled step was proton-independent electron transfer process, with minimal impact from substrate concentration variations. After assembling synchronous reaction cell, PERO generated yields DHMF (94%) FDCA (86%), combined 131%, doubling performance uncoupled cells. This superior attributed efficient generation H* alloy reduction, alongside OH* active sites electrode oxidation. research provides promising strategy sustainable upgrading chemicals.

Language: Английский

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Novel photoelectrocatalytic system of oxygen vacancy-rich black TiO2-x nanocones photoanode and natural air diffusion cathode for efficient water purification and simultaneous H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 124042 - 124042

Published: April 21, 2024

Language: Английский

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Tandem Integration of Biological and Electrochemical Catalysis for Efficient Polyester Upcycling under Ambient Conditions

Nano Letters, Journal Year: 2024, Volume and Issue: 24(31), P. 9768 - 9775

Published: July 26, 2024

Excessive production of waste polyethylene terephthalate (PET) poses an ecological challenge, which necessitates developing technologies to extract the values from end-of-life PET. Upcycling has proven effective in addressing low profitability current recycling strategies, yet existing upcycling operate under energy-intensive conditions. Here we report a cascade strategy steer transformation PET into glycolate overall yield 92.6% ambient The approach involves setting up robust hydrolase with 95.6% depolymerization ethylene glycol (EG) monomer within 12 h, followed by electrochemical process initiated CO-tolerant Pd/Ni(OH)

Language: Английский

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Rationally Designed Carbon‐Based Catalysts for Electrochemical C‐N Coupling

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(28)

Published: May 7, 2024

Abstract The electrochemical C‐N coupling process, facilitating the production of organic nitrogen substances (such as urea, methylamine, formamide, and ethylamine) via simultaneous reduction carbon dioxide (CO 2 ) small nitrogen‐based substances, stands at forefront advancing neutrality artificial cycle. This method has garnered substantial interest due to its potential economic environmental benefits. Although considerable progress been achieved in this emerging field, it still faces challenges, including slow reactant adsorption, competing side reactions, complex multi‐step pathways, resulting low yields selectivity. Strategically designing developing low‐cost exceptionally performant catalysts is crucial for cost‐effective precise C─N bonding. article offers an in‐depth review electrosynthesis valuable compounds ambient conditions from earth‐abundant resources/wastes, such CO nitrogenous molecules (nitrogen: N , nitrite: NO − nitrate: 3 ammonia: NH etc.), bond formation especially using carbon‐based catalysts. relevant mechanisms, design principles advanced electrocatalysts, impact different electrolyser designs are discussed, along with present obstacles upcoming prospects dynamic field.

Language: Английский

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Fe-based “electron pump” involving NiCo-LDH enables robust and highly-selective electrocatalytic methanol oxidation to formic acid

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(5), P. 2638 - 2644

Published: Jan. 1, 2024

Nucleophile oxidation reactions, represented by the incomplete methanol reaction (i-MOR) to formic acid, can effectively lower potential of electrolytic hydrogen production while generating high-value products.

Language: Английский

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Metal-organic frameworks as thermocatalysts for hydrogen peroxide generation and environmental antibacterial applications

Science Advances, Journal Year: 2025, Volume and Issue: 11(2)

Published: Jan. 8, 2025

Reactive oxygen species (ROS) are highly reactive, making them useful for environmental and health applications. Traditionally, photocatalysts piezocatalysts have been used to generate ROS, but their utilization is limited by various physical constraints. This study introduces metal-organic frameworks (MOFs) as modern thermocatalysts efficiently producing hydrogen peroxide (H 2 O ) from small temperature differences. Temperature fluctuations, abundant in daily life, offer tremendous potential practical thermocatalytic As proof of concept, MOF materials coated onto carbon fiber fabric (MOF@CFF) created a antibacterial filter. The compared three different MOFs (CuBDC, MOF-303, ZIF-8) with bismuth telluride (Bi Te 3 ), known material. ZIF-8 demonstrated superior H generation under low-temperature differences, achieving 96% activity through variation cycles. work advances thermoelectric applications MOFs, enabling real-time purification disinfection generation. findings open interdisciplinary avenues leveraging effects catalysis technologies.

Language: Английский

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Engineering Asymmetric Electronic Structure of Co─N─C Single‐Atomic Sites Toward Excellent Electrochemical H₂O₂ Production and Biomass Upgrading

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract To advance electrochemical H 2 O production and unravel catalytic mechanisms, the precise structural coordination of single‐atomic M‐N‐C electrocatalysts is urgently required. Herein, Co─N 5 site with an asymmetric electronic configuration constructed to boost two‐electron oxygen reduction reaction (2e − ORR) compared symmetric 4 , effectively overcoming trade‐off between activity selectivity in production. Both experimental theoretical analyses demonstrate that breaking symmetry sites promotes activation molecules moderates adsorption key *OOH intermediate by disrupting linear scaling relationship for intermediates adsorption. This modulation enables efficient H₂O₂ its effective retention subsequent applications. As a proof concept, achieves rate as high 16.1 mol g cat −1 h flow cell, outperforming most recently reported counterparts. Furthermore, coupling 2e ORR oxidation cellulose‐derived carbohydrates accomplishes formic acid yields (84.1% from glucose 62.0%–92.1% other substrates), underpinning sustainable electro‐refinery biomass valorization at ambient conditions. By elucidating intrinsic 2e⁻ asymmetry sites, this work paves way high‐performance electrosynthesis.

Language: Английский

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