Multifunctional carbon nitride nanoarchitectures for catalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7602 - 7664

Published: Jan. 1, 2023

Carbon nitrides, with feasibility of tailored band gap via suitable nanoarchitectonics, are deemed as best catalysts amongst existing materials, especially for HER, OWS, COR, NRR, water oxidation, pollutant removal, and organocatalysis.

Language: Английский

---

Recent developments in heterogeneous electrocatalysts for ambient nitrogen reduction to ammonia: Activity, challenges, and future perspectives

Renewable and Sustainable Energy Reviews, Journal Year: 2023, Volume and Issue: 176, P. 113197 - 113197

Published: Feb. 2, 2023

Language: Английский

---

Enhancing polyol/sugar cascade oxidation to formic acid with defect rich MnO2 catalysts

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

Published: July 26, 2023

Oxidation of renewable polyol/sugar into formic acid using molecular O2 over heterogeneous catalysts is still challenging due to the insufficient activation both and organic substrates on coordination-saturated metal oxides. In this study, we develop a defective MnO2 catalyst through coordination number reduction strategy enhance aerobic oxidation various polyols/sugars acid. Compared common MnO2, tri-coordinated Mn in displays electronic reconstruction surface oxygen charge state rich vacancies. These vacancies create more Mnδ+ Lewis site together with nearby as base sites. This combined structure behaves much like Frustrated pairs, serving facilitate O2, well C-C C-H bonds. As result, shows high catalytic activity (turnover frequency: 113.5 h-1) yield (>80%) comparable noble for glycerol oxidation. The system further extended other excellent performance.

Language: Английский

---

Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering

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

Published: Oct. 7, 2023

Hydrogen peroxide (H

Language: Английский

---

Unexpected Energy Applications of Ionic Liquids

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(23)

Published: Feb. 27, 2024

Ionic liquids and their various analogues are without doubt the scientific sensation of last few decades, paving way to a more sustainable society. Their versatile suite properties, originating from an almost inconceivably large number possible cation anion combinations, allows tuning structure serve desired purpose. hence offer myriad useful applications solvents catalysts, through lubricants, gas absorbers, azeotrope breakers. The purpose this review is explore unexpected these applications, particularly in energy space. It guides reader application ionic as i) phase change materials for thermal storage, ii) organic plastic crystals, which have been studied battery electrolytes separation, iii) key components nitrogen reduction reaction ammonia generation, iv) aluminum-ion batteries, v) other emerging technologies. concluded that there tremendous scope further optimizing liquid its task, subject sustainability imperatives line with current global priorities, assisted by artificial intelligence.

Language: Английский

---

Atomic-level reactive sites for electrocatalytic nitrogen reduction to ammonia under ambient conditions

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 489, P. 215196 - 215196

Published: May 10, 2023

Language: Английский

---

Investigating High-Performance Non-Precious Transition Metal Oxide Catalysts for Nitrogen Reduction Reaction: A Multifaceted DFT–kMC–LSTM Approach

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(13), P. 8336 - 8346

Published: June 8, 2023

The need for non-precious-metal catalysts the nitrogen reduction reaction (NRR) is growing due to high cost of precious-metal catalysts. Transition metal oxides (TMOs) are a promising option, but there limited experimental and computational evidence their use. present work comprehensive investigation multiple TMOs utilizing multifaceted approach. Specifically, we integrated density functional theory (DFT) analyze thermodynamic electronic properties, kinetic Monte Carlo (kMC) simulate entire pathway candidate materials, long–short-term memory (LSTM) methods incorporate long-term surface degradation within model. Using this approach, predicted that V2O3 would exhibit superior NRR activity compared noble Ru catalyst, with turnover frequency 1000 times higher, while also demonstrating stable performance over 10,000 h. It noteworthy one key factors contributing unique ability upshift O 2p-band tensile strain generated by N2-TM site binding. This allows swift H transfer adjacent N-containing species on TM sites weakening binding strength, leading an accelerated process. Overall, provides holistic through DFT–kMC–LSTM approach demonstrates leverage complementary between rather than suppressing competing hydrogen evolution (HER) processes.

Language: Английский

---

Visible-Light Photocatalytic H₂O₂ Production Boosted by Frustrated Lewis Pairs in Defected Polymeric Carbon Nitride Nanosheets

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(4), P. 2775 - 2786

Published: Feb. 7, 2024

Frustrated Lewis pairs (FLPs) with a unique "push–pull" effect can effectively activate many types of molecules to obtain unanticipated catalytic activity. Herein, FLPs are introduced into polymeric carbon nitride (CN), and their functions in the photocatalytic synthesis H2O2 studied. The B-doped CN (BCN) constituted by electron-deficient boron as acid sites nitrogen neighbored cyano groups base sites. formation improve light absorption ability separation photogenerated carriers. afford strong adsorption O2, but cannot produce directly because activation oxygen bonds leads bond scission during reduction. enhance production through effective ethanol (ETOH) FLPs. reduction O2 is found •O2– 1O2 species. rate on BCN reach 51,008 μM g–1 h–1, which over 12 times that pristine (4113 h–1). This study not only provides an approach for enhancing also deepens understanding role molecule activation.

Language: Английский

---

Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers

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

Published: May 31, 2024

Abstract Adsorption and activation of C–H bonds by photocatalysts are crucial for the efficient conversion to produce high-value chemicals. Nevertheless, delivery surface-active oxygen species bond oxygenation inevitably needs overcome obstacles due separated active centers, which suppresses catalytic efficiency. Herein, Ni dopants introduced into a monolayer Bi 2 WO 6 create cascaded units consisting unsaturated W atoms Bi/O frustrated Lewis pairs. Experimental characterizations density functional theory calculations reveal that these special sites can establish an controllable oxidation process. The activated on readily transferred oxygenation. catalyst with mass fraction 1.8% exhibits excellent toluene rates high selectivity towards benzaldehyde. This study presents fascinating strategy through design units.

Language: Английский

---

Efficient Homolytic Cleavage of H₂O₂ on Hydroxyl‐Enriched Spinel CuFe₂O₄ with Dual Lewis Acid Sites

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 1, 2024

Abstract Traditional H 2 O cleavage mediated by macroscopic electron transfer (MET) not only has low utilization of , but also sacrifices the stability catalysts. We present a non‐redox hydroxyl‐enriched spinel (CuFe 4 ) catalyst with dual Lewis acid sites to realize homolytic . The results systematic experiments, in situ characterizations, and theoretical calculations confirm that tetrahedral Cu optimal acidity strong delocalization can synergistically elongate O−O bonds (1.47 Å → 1.87 Å) collaboration adjacent bridging hydroxyl (another site). As result, free energy is decreased (1.28 eV 0.98 eV). be efficiently split into ⋅OH induced CuFe without MET, which greatly improves (65.2 %, nearly times than traditional catalysts). system assembled affords exceptional performance for organic pollutant elimination. scale‐up experiment using continuous flow reactor realizes long‐term (up 600 mL), confirming tremendous potential practical applications.

Language: Английский

---