Flexible Single‐Atom Cesium Sites on Amorphous MgO Nano‐Cushions for Enhanced CO2‐Involved Multi‐Step Reactions DOI

Qiuyan Cao,

Wenqiang Sun, Zhen Yin

и другие.

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 24, 2025

Abstract Single atomic sites (SAs) face challenges in catalyzing complex chemical processes involving multiple intermediates due to rigid coordination environments, steric hindrances, and limited activation behaviors. Herein, an alloying‐mediated element repartition method is developed synthesize flexible cesium single‐atom catalysts, anchoring Cs single on precisely controlled amorphous‐MgO/crystalline NbC hetero‐phase nano‐supports. The amorphousMgO(a‐MgO) equipped 1 ‐a‐MgO/NbC achieves 91% yield the cyclization of CO 2 with 2‐aminobenzonitrile within a gas–liquid–solid triphasic system, outperforming its counterpart fabricated crystalline MgO, ‐c‐MgO/NbC catalyst (only 23%). shows excellent tolerance various functional groups sustainable catalysis, especially removing traditional requirement for high‐pressure conditions additives. Operando spectroscopic characterizations theoretical calculations demonstrate that sandwich‐structural enhances consecutive through vertically adsorbed configurations during C‐N coupling N‐heterocyclic ring formation. SAs supported by a‐MgO nano‐cushions allow adaptability dynamic transformations via tensile Cs‐O compressive Mg─O bonds, ultimately reducing energy barriers critical rearrangement isomerization steps. This study provides valuable insights into designing SACs overcome limitations support interfaces, thereby enhancing performance toward multi‐intermediate conversion heterogeneous catalytic transformations.

Язык: Английский

Cuδ+ Site-Enhanced Adsorption and Crown Ether-Reconfigured Interfacial D2O Promote Electrocatalytic Dehalogenative Deuteration DOI
Meng He, Haotian Wang, Chuanqi Cheng

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 28, 2025

Electrocatalytic dehalogenative deuteration is a sustainable method for precise deuteration, whereas its Faradaic efficiency (FE) limited by high overpotential and severe D2 evolution reaction (DER). Here, Cuδ+ site-adjusted adsorption crown ether-reconfigured interfacial D2O are reported to cooperatively increase the FE of up 84% at −100 mA cm–2. sites strengthen aryl iodides, promoting mass transfer thus accelerating kinetics toward deuteration. The ethers disrupt hydration effect K·D2O reconstruct hydrogen bond with D2O, lowering content electric double layer hindering interaction between cathode, inhibiting competitive DER. A linear relationship matched sizes alkali metal cations demonstrated universally increasing FEs. This also suitable various halides easily reducible functional group compatibility improved FEs

Язык: Английский

Процитировано

2
Bimetallic effects in the carbon dioxide electroreduction DOI Creative Commons

Anaer Husile,

Zhenlü Wang, Jingqi Guan

и другие.

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review systematically summarizes the latest advances in bimetallic effects for reduction of CO 2 to multi-carbon products, discussing structure–activity relationships typical catalysts reaction.

Язык: Английский

Процитировано

2
High‐Entropy Materials: from Bulk to Sub‐nano DOI Open Access

Xiaoya Wang,

Qingda Liu, Xun Wang

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 12, 2025

Abstract High‐entropy materials (HEMs), characterized by their unique compositions involving multiple principal elements and inherent configurational disorder, have emerged as a focal point of material science research since introduction, owing to exceptional structural stability superior performance. The distinctive features HEMs, including the high‐entropy effect, lattice distortion, sluggish diffusion, cocktail enabled wide‐ranging applications in fields such energy storage, catalysis, electronic devices, beyond. This review systematically documents evolution HEMs synthesis, from traditional melting‐based methods for bulk production recent breakthroughs addressing limitations elemental immiscibility, ultimately enabling precise multi‐path synthesis nano‐ sub‐nano materials. It comprehensively examines controllable strategies across various dimensional scales, principles composition‐structure design, regulation multidimensional morphologies, multifunctional properties materials' multi‐component characteristics. Furthermore, this work prospectively explores emerging that could drive future development with particular emphasis on potential synergies between high‐throughput experimentation, data‐driven approaches, chiral factors, entropy‐driven strategies, advanced high‐resolution characterization techniques.

Язык: Английский

Процитировано

1
Density Functional Theory Simulations of Skaergaardite (CuPd) with a Self-Consistent Hubbard U-Correction DOI Creative Commons
Martino Napoli, Assimo Maris

Chemistry, Год журнала: 2025, Номер 7(2), С. 56 - 56

Опубликована: Апрель 2, 2025

The electronic and phonon bands of Skaergaardite are investigated using density functional theory (DFT) as implemented in Quantum ESPRESSO. is a copper palladium mineral (CuPd) found the Skaergaard intrusion with CsCl-type (B2) structure. Due to its porous structure, it presents large surface area available for interactions, which makes promising catalyst. PBE-GGA Hubbard-like localized term (DFT+U) combined ultrasoft norm-conserving pseudopotentials, conventional approach dense Monkhorst–Pack grid k-points 12 × applied. valence mainly constituted by 3d orbitals Cu 4d Pd pseudo-gap can be recognized. With respect DFT, DFT+U causes general downward shift band. acoustic optical branches separated few cm−1 gap at about 150 show state curve typical ordered materials. These results highlight reliability studying bimetallic systems scarce experimental benchmarks, offering insights into behavior potential applications material science such reduction reactions hydrogen storage.

Язык: Английский

Процитировано

0
Promoting CO2 electroreduction to C2H4 product by promoting water molecules activation on MgO/CuO catalyst DOI

Mengyao Feng,

Zhichao Chen,

Hanlei Sun

и другие.

Journal of Energy Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Апрель 1, 2025

Язык: Английский

Процитировано

0
Flexible Single‐Atom Cesium Sites on Amorphous MgO Nano‐Cushions for Enhanced CO2‐Involved Multi‐Step Reactions DOI

Qiuyan Cao,

Wenqiang Sun, Zhen Yin

и другие.

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 24, 2025

Abstract Single atomic sites (SAs) face challenges in catalyzing complex chemical processes involving multiple intermediates due to rigid coordination environments, steric hindrances, and limited activation behaviors. Herein, an alloying‐mediated element repartition method is developed synthesize flexible cesium single‐atom catalysts, anchoring Cs single on precisely controlled amorphous‐MgO/crystalline NbC hetero‐phase nano‐supports. The amorphousMgO(a‐MgO) equipped 1 ‐a‐MgO/NbC achieves 91% yield the cyclization of CO 2 with 2‐aminobenzonitrile within a gas–liquid–solid triphasic system, outperforming its counterpart fabricated crystalline MgO, ‐c‐MgO/NbC catalyst (only 23%). shows excellent tolerance various functional groups sustainable catalysis, especially removing traditional requirement for high‐pressure conditions additives. Operando spectroscopic characterizations theoretical calculations demonstrate that sandwich‐structural enhances consecutive through vertically adsorbed configurations during C‐N coupling N‐heterocyclic ring formation. SAs supported by a‐MgO nano‐cushions allow adaptability dynamic transformations via tensile Cs‐O compressive Mg─O bonds, ultimately reducing energy barriers critical rearrangement isomerization steps. This study provides valuable insights into designing SACs overcome limitations support interfaces, thereby enhancing performance toward multi‐intermediate conversion heterogeneous catalytic transformations.

Язык: Английский

Процитировано

0