Direct Electrosynthesis of Urea from Carbon Dioxide and Nitric Oxide

ACS Energy Letters, Journal Year: 2021, Volume and Issue: 7(1), P. 284 - 291

Published: Dec. 15, 2021

Electrochemical synthesis of urea provides a sustainable strategy that can be easily incorporated into currently distributed renewable energy systems. The main challenge hindered the advancement this technique lies in developing advanced electrocatalytic processes to utilize abundant and low-cost inorganic carbon nitrogen sources for highly productive generation. Herein, we report an reaction converts dioxide (CO2) nitric oxide (NO) urea, with water as hydrogen source, under ambient conditions. yield rate Faradaic efficiency reach 15.13 mmol g–1 h–1 11.26% at current density 40 mA cm–2 optimized critical intermediates *CO *NH2 generation are obtained via co-reduction CO2 NO then continuously interconnect form C–N bond. A preliminary techno-economic study is performed discuss practical application potential production.

Language: Английский

---

Electrocatalytic Hydrogenation of 5‐Hydroxymethylfurfural Promoted by a Ru₁Cu Single‐Atom Alloy Catalyst

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(37)

Published: July 25, 2022

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) represents an elegant route toward sustainable value-added chemicals production that circumvents the use fossil fuel and hydrogen. However, reaction efficiency is hampered by high voltage low activity electrodes (Cu, Bi, Pb). Herein, we report a Ru1 Cu single-atom alloy (SAA) catalyst with isolated Ru atoms on nanowires exhibits electrochemical HMF to 2,5-dihydroxymethylfuran (DHMF) promoted productivity (0.47 vs. 0.08 mmol cm-2 h-1 ) faradic (FE) (85.6 71.3 %) at -0.3 V (vs. RHE) compared counterpart. More importantly, FE (87.5 largely retained concentration (100 mM). Kinetic studies using combined techniques suggest disparate mechanisms over Cu, revealing promotes dissociation water produce H* species effectively react via electrocatalytic hydrogenation (ECH) mechanism.

Language: Английский

---

Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 49 - 113

Published: Nov. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Language: Английский

---

Electrocatalytic Valorization of Poly(ethylene terephthalate) Plastic and CO₂ for Simultaneous Production of Formic Acid

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(11), P. 6722 - 6728

Published: May 23, 2022

The electro-reforming of polymer plastic waste and CO2 has the merits for producing value-added chemicals alleviating environmental pollution. Herein, we report an electrocatalytic integrating strategy efficient valorization poly(ethylene terephthalate) (PET) to simultaneously produce formic acid at both anode cathode. NiCo2O4 electrocatalyst displays a high Faradaic efficiency 90% production, which indicates excellent selectivity PET hydrolysate oxidation. By coupling oxidation reaction with reduction reaction, assembled electrolyzer exhibits low cell voltage 1.55 V drive integrated two half-reactions. Furthermore, 155% can be achieved 1.90 V. This study suggests that could energy-efficient economically viable realize production chemicals.

Language: Английский

---

Promoting biomass electrooxidation via modulating proton and oxygen anion deintercalation in hydroxide

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: June 30, 2022

Abstract The redox center of transition metal oxides and hydroxides is generally considered to be the site. Interestingly, proton oxygen in lattice recently are found actively involved catalytic reactions, critically determine reactivity. Herein, taking glycerol electrooxidation reaction as model reaction, we reveal systematically impact anion (de)intercalation processes on elementary steps. Combining density functional theory calculations advanced spectroscopy techniques, find that doping Co into Ni-hydroxide promotes deintercalation from catalyst surface. vacancies formed NiCo hydroxide during increase d -band filling sites, facilitating charge transfer surface cleaved molecules 2 nd C-C bond cleavage. Consequently, exhibits enhanced activity, with a current 100 mA/cm at 1.35 V formate selectivity 94.3%.

Language: Английский

---

Atomically Dispersed Pt–N₃C₁ Sites Enabling Efficient and Selective Electrocatalytic C–C Bond Cleavage in Lignin Models under Ambient Conditions

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(25), P. 9429 - 9439

Published: June 17, 2021

Selective cleavage of C–C linkages is the key and a challenge for lignin degradation to harvest value-added aromatic compounds. To this end, electrocatalytic oxidation presents promising technique by virtue mild reaction conditions strong sustainability. However, existing electrocatalysts (traditional bulk metal oxides) bond oxidative suffer from poor selectivity low product yields. We show first time that atomically dispersed Pt–N3C1 sites planted on nitrogen-doped carbon nanotubes (Pt1/N-CNTs), constructed via stepwise polymerization–carbonization–electrostatic adsorption strategy, are highly active selective toward Cα–Cβ in β-O-4 model compounds under ambient conditions. Pt1/N-CNTs exhibits 99% substrate conversion with 81% yield benzaldehyde, which exceptional unprecedented compared previously reported electrocatalysts. Moreover, using only 0.41 wt % Pt achieved much higher benzaldehyde than those state-of-the-art electrode (100 Pt) commercial Pt/C catalyst (20 Pt). Systematic experimental investigation together density functional theory (DFT) calculation suggests superior performance arises facilitating formation Cβ radical intermediate, further inducing radical/radical cross-coupling path break bond. This work opens up opportunities valorization green sustainable electrochemical route ultralow noble usage.

Language: Английский

---

Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(6), P. 2193 - 2237

Published: Jan. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Language: Английский

---

High-entropy alloys in electrocatalysis: from fundamentals to applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8319 - 8373

Published: Jan. 1, 2023

In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.

Language: Английский

---

Integrated Catalytic Sites for Highly Efficient Electrochemical Oxidation of the Aldehyde and Hydroxyl Groups in 5-Hydroxymethylfurfural

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(7), P. 4242 - 4251

Published: March 23, 2022

5-Hydroxymethylfurfural oxidation reaction (HMFOR) is regarded as a promising approach to attain biomass-derived high-value chemical products. As the HMFOR process complicated, and two-step of aldehyde group hydroxyl in 5-hydroxymethylfurfural (HMF) typically involved, it fundamentally significant understand different catalytic processes for HMFOR. In this work, we identify direct synergistic types on cobalt oxide catalysts. For process, Co3O4 was found have higher activity than due barrier hydration oxidation. By studying behaviors transition metal oxides, NiO exhibited optimal owing appropriate OH adsorption energy alcohol dehydrogenation. Therefore, performance achieved by accurately introducing Ni into tetrahedral sites spinel oxides improve activity. The integrated enhanced overall with 92.42% FDCA yield 90.35% faradaic efficiency. This work provides perspective designing efficient electrocatalysts

Language: Английский

---

A dynamic Ni(OH)2-NiOOH/NiFeP heterojunction enabling high-performance E-upgrading of hydroxymethylfurfural

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 311, P. 121357 - 121357

Published: March 28, 2022

Language: Английский

---