Using a Single-Atom FeN4 Catalyst on Defective Graphene for the Efficient Reduction of NO to Alanine: A Computational Study DOI Open Access
Yu Tian, Xiaoxi Yuan,

Zexuan Guo

и другие.

Catalysts, Год журнала: 2024, Номер 14(12), С. 876 - 876

Опубликована: Ноя. 30, 2024

The use of a single-atom FeN4 catalyst on defective graphene (Fe-NC) has recently emerged as an effective method for the synthesis amino acids. Herein, we investigated mechanism alanine formation FeN4-doped using comprehensive density functional theory (DFT) computations. reaction begins with activation NO molecules surface, followed by their hydrogen atoms provided in system. computational results show that can be effectively activated Fe-NC, facilitating subsequent at relatively lower potential. potential-limiting step production involves either HNO* or HNOH* intermediates Fe-NG, free energy changes (ΔG) these two elementary steps are nearly equivalent. Notably, exhibits higher (Ea) compared to formation. This study provides valuable insights into C–N coupling and acid catalysts.

Язык: Английский

Recent Advances on Carbon‐Based Metal‐Free Electrocatalysts for Energy and Chemical Conversions DOI Creative Commons
Qingfeng Zhai,

Hetaishan Huang,

Tom Lawson

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 25, 2024

Over the last decade, carbon-based metal-free electrocatalysts (C-MFECs) have become important in electrocatalysis. This field is started thanks to initial discovery that nitrogen atom doped carbon can function as a electrode alkaline fuel cells. A wide variety of nanomaterials, including 0D dots, 1D nanotubes, 2D graphene, and 3D porous carbons, has demonstrated high electrocatalytic performance across applications. These include clean energy generation storage, green chemistry, environmental remediation. The applicability C-MFECs facilitated by effective synthetic approaches, e.g., heteroatom doping, physical/chemical modification. methods enable creation catalysts with properties useful for sustainable transformation storage (e.g., cells, Zn-air batteries, Li-O

Язык: Английский

Процитировано

28

Purification and Value-Added Conversion of NOx under Ambient Conditions with Photo-/Electrocatalysis Technology DOI

Ruimin Chen,

Jielin Wang, Chunling Zhang

и другие.

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 6, 2025

As primary air pollutants from fossil fuel combustion, the excess emission of nitric oxides (NOx) results in a series atmospheric environmental issues. Although selective catalytic reduction technology has been confirmed to be effective for NOx removal, green purification and value-added conversion under ambient conditions are still facing great challenges, especially nitrogen resource recovery. To address that, photo-/electrocatalysis offers sustainable routes efficient upcycling temperature pressure, which received considerable attention scientific communities. In this review, recent advances critically summarized. The target products reaction mechanisms systems, together with responsible active sites, discussed, respectively. Then, realistic practicability is proposed, including strict performance evaluation criteria application by photo-/electrocatalysis. Finally, current challenges future opportunities proposed terms catalyst design, enhancement, mechanism understanding, practical conditions, product separation techniques.

Язык: Английский

Процитировано

2

Selective Synthesis of Organonitrogen Compounds via Electrochemical C–N Coupling on Atomically Dispersed Catalysts DOI
Yang Liu, Xiao-Yong Yu, Xintong Li

и другие.

ACS Nano, Год журнала: 2024, Номер 18(35), С. 23894 - 23911

Опубликована: Авг. 20, 2024

The C-N coupling reaction demonstrates broad application in the fabrication of a wide range high value-added organonitrogen molecules including fertilizers (e.g., urea), chemical feedstocks amines, amides), and biomolecules amino acids). electrocatalytic pathways from waste resources like CO

Язык: Английский

Процитировано

9

Multifunctional Carbon‐Based Metal‐Free Catalysts for Cascade Electrochemical‐Chemical Coupling Catalyses DOI Open Access
Yan Li, Tom Lawson,

Yang Hou

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 10, 2025

Abstract Cascade electrochemical‐chemical coupling (CECC) involves sequential electrochemical and chemical reactions, using intermediates from processes as reactants for subsequent transformations to enhance the efficiency selectivity sustainable syntheses of complex chemicals. Despite its economic environmental benefits, CECC still faces multiple challenges, including a low utilization intermediate reactants, competitive side difficulties in design scale‐up catalysts, leading yield. To ensure economically viable CECC, it is imperative rationally develop cost‐efficient high‐performance such carbon‐based metal‐free electrocatalysts (C‐MFECs) certain carbon‐supported transition metal with high activity atomic precision desirable products. In this review, an overview recent advancements doping C‐MFECs provided enhancing their catalytic toward CECC. Three major systems based on are discussed; they hydrogen peroxide coupling, carbon dioxide upgrading, redox‐mediated systems. Current challenges future perspectives emerging field also addressed.

Язык: Английский

Процитировано

1

Stabilization of Cuδ+ Sites Within MnO2 for Superior Urea Electro‐Synthesis DOI Open Access
Yidong Yang,

Guanzheng Wu,

Jiadi Jiang

и другие.

Advanced Materials, Год журнала: 2024, Номер 36(41)

Опубликована: Сен. 2, 2024

Abstract Electrocatalytic C‐N coupling between NO 3 ‐ and CO 2 has emerged as a sustainable route for urea production. However, identifying catalytic active sites designing efficient electrocatalysts remain significant challenges. Herein, the synthesis of Cu‐doped MnO nanotube (denoted Cu‐MnO ) with stable Cu δ+ ‐oxygen vacancies (O vs )‐Mn 3+ dual is reported. Compared pure , doping can effectively enhance production performance in co‐reduction . Thus, catalyst exhibits maximum Faradaic efficiency (FE) 54.7% highest yield rate 116.7 mmol h −1 g cat. flow cell. Remarkably, remains over 78 across wide potential range. Further experimental theoretical results elucidate unique role solid‐solution stabilizing ‐O ‐Mn endowing superior structural electrochemical stabilities. This thermodynamically promotes formation kinetically lowers energy barrier coupling.

Язык: Английский

Процитировано

5

Electrocatalytic and Photocatalytic N2 Fixation Using Carbon Catalysts DOI Creative Commons
Changchun Xu, Hongli Su, Shuaifei Zhao

и другие.

Nanomaterials, Год журнала: 2025, Номер 15(1), С. 65 - 65

Опубликована: Янв. 2, 2025

Carbon catalysts have shown promise as an alternative to the currently available energy-intensive approaches for nitrogen fixation (NF) urea, NH3, or related nitrogenous compounds. The primary challenges NF are natural inertia of molecules and competitive hydrogen evolution reaction (HER). Recently, carbon-based materials made significant progress due their tunable electronic structure ease defect formation. These properties significantly enhance electrocatalytic photocatalytic reduction (NRR) activity. While transition metal-based solved kinetic constraints activate bonds via donation-back-π approach, there is a problem: d-orbital electrons these metal atoms tend generate H-metal bonds, inadvertently amplifying unwanted HER. Because this, timely review defective electrocatalysts imperative. Such will succinctly capture recent developments in both experimental theoretical fields. It delve into multiple engineering advance development ideal photocatalysts. Furthermore, this carefully explore correlation between photocatalysts Finally, novel introduced obtain more efficient performance NF, paving way sustainable future.

Язык: Английский

Процитировано

0

Tuning the CO2 and CO Electroreduction by Rate-Determining and Selectivity-Determining Steps DOI

Yuanyuan Xue,

Lijuan Zhang,

Min Kuang

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

The renewable electricity-driven CO2 and CO reduction represents a promising approach for reducing the footprint toward carbon neutrality. Substantial research developments have been achieved in designing catalysts reaction interfaces enhanced electrocatalytic activity selectivity, investigation understanding of complex mechanisms also extensively investigated by both situ characterizations theoretical investigations. Although quasi-equilibrium rate-determining step assumptions are widely used electrochemical kinetics, overall rate is generally determined series elementary steps, influence certain can be quantified based on degree control theory. For complicated networks CO(2) reduction, not only steps but subsequent selectivity-determining play critical roles, especially product selectivity. In this Perspective, we summarize strategies that tune selectivity their impacts respectively. addition, describe coupling electroreduction with other (electro)chemical reactions, such as nitrite methane oxidation, to form value-added products. At end, current challenges opportunities field discussed inspire further development next stage.

Язык: Английский

Процитировано

0

Dual Activation of N2 and CO2 toward N–O Coupling by Single Copper Ions DOI

Qiuhao Yi,

Chaonan Cui,

Demiao Ma

и другие.

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Фев. 18, 2025

Concurrent activation and conversion of N2 CO2 are significance yet face numerous obstacles due to the large dissociation energies N≡N C═O bonds. Utilizing a specifically developed reflectron time-of-flight mass spectrometer, we investigated dual mediated by copper silver ions under ambient conditions. Isotope experiments identified that both can be effectively activated generate N–O coupling product (NO+), especially in presence ions, NO+ attains maximum intensity with an N2/CO2 ratio 1:2, which validates three-molecule reaction mechanism, namely, + 2CO2 → 2NO 2CO. Through detailed analyses thermo-dynamics dynamics, illustrate Cu+-catalyzed mechanism for coupling, validating simply plasma-assisted single-ion catalysis.

Язык: Английский

Процитировано

0

Co-Embedding homonuclear Dual-Metal sites and phosphorus atom to achieve efficient methylamine electrosynthesis from carbon dioxide and nitrate DOI
Ao Yang, Changyan Zhu,

Kaile Li

и другие.

Applied Surface Science, Год журнала: 2025, Номер 700, С. 163194 - 163194

Опубликована: Апрель 10, 2025

Язык: Английский

Процитировано

0

Carbon-based nanomaterials for carbon neutralization through electrochemical CO2 reduction and C–N coupling DOI
Tanglue Feng,

Jinze Yang,

Jiajia Huang

и другие.

Matter, Год журнала: 2025, Номер 8(5), С. 102077 - 102077

Опубликована: Май 1, 2025

Язык: Английский

Процитировано

0