Multifunctional carbon nitride nanoarchitectures for catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 52(21), С. 7602 - 7664

Опубликована: Янв. 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.

Язык: Английский

---

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

Renewable and Sustainable Energy Reviews, Год журнала: 2023, Номер 176, С. 113197 - 113197

Опубликована: Фев. 2, 2023

Язык: Английский

---

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

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Июль 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.

Язык: Английский

---

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

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Окт. 7, 2023

Hydrogen peroxide (H

Язык: Английский

---

Unexpected Energy Applications of Ionic Liquids

Advanced Materials, Год журнала: 2024, Номер 36(23)

Опубликована: Фев. 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.

Язык: Английский

---

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

Coordination Chemistry Reviews, Год журнала: 2023, Номер 489, С. 215196 - 215196

Опубликована: Май 10, 2023

Язык: Английский

---

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

ACS Catalysis, Год журнала: 2024, Номер 14(4), С. 2775 - 2786

Опубликована: Фев. 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.

Язык: Английский

---

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

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)

Опубликована: Март 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.

Язык: Английский

---

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

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Май 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.

Язык: Английский

---

Progress in Single/Multi Atoms and 2D‐Nanomaterials for Electro/Photocatalytic Nitrogen Reduction: Experimental, Computational and Machine Leaning Developments

Advanced Energy Materials, Год журнала: 2024, Номер 14(28)

Опубликована: Фев. 11, 2024

Abstract The conversion of atmospheric nitrogen (N 2 ) into ammonia (NH 3 ), known as fixation, plays a crucial role in sustaining life on Earth, facing innovation with electrocatalytic and photocatalytic methods. These approaches promise gentler conversions from to ammonia, diverging the energy‐intensive Haber‐Bosch process, which requires complex plant infrastructure. Vitality lies eco‐friendly, cost‐effective, energy‐efficient pathways. challenge is that electrocatalysts photocatalysts for reduction have shown low Faraday efficiency, hampered by hydrogen evolution. This work delves recent strides electro/photo‐catalytic fixation/reduction, deciphering mechanisms, catalysts, prospects. By unveiling core principles steering these processes, it dissects efficiency drivers. Experimental theoretical studies, ranging density functional calculations/simulations machine learning‐based catalyst screening, mark path toward highly efficient including single/multi‐atom catalysts embedded 2D materials. journey explores diverse assessing their performance, spotlighting emerging nanomaterials, heterostructures, co‐catalyst techniques. Perspectives future directions potential applications fixation/reduction are offered, emphasizing sustainable management implications global agriculture environmental sustainability.

Язык: Английский

---