Molecular Dynamics Simulations for Electrocatalytic CO2 Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms DOI
Yanzheng He, Mengfan Wang, Haoqing Ji

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 6, 2024

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) has been recognized as a promising route to convert emissions high‐value chemicals and fuels. Significant breakthroughs are usually inseparable from deeper understanding of mechanisms. To this end, molecular dynamics (MD) simulations have invaluable in providing detailed insights into elucidation complex pathways prediction overall electrochemical performance, thus bridging macroscopic experimental observations microscopic explanatory Directed by MD simulations, tremendous efforts devoted toward enhancing the CO RR with rational design electrocatalyst efficient construction electrode/electrolyte interface. Herein, comprehensive review applications is emerged. begin with, specific fundamentals along familiar methods such algorithm force fields various summed up. Followed, employment optimization introduced, encompassing interpretation activity, explanation electrolyte effect, investigation electrode microenvironment. Definitively, imminent challenges avenues for future contemplated, envisioning guiding beacon endeavors aimed at harnessing propel realm heightened efficiency, economic viability, practical utility.

Язык: Английский

Quaternary Medium-Entropy Alloy Metallene with Strong Charge Polarization for Highly Selective Urea Electrosynthesis from Carbon Dioxide and Nitrate DOI
Yuanbo Zhou, Mengfan Wang, Lifang Zhang

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Фев. 14, 2025

Electrochemical urea synthesis via the coreduction of CO2 and NO3- is a sustainable alternative to traditional Bosch-Meiser process. However, sluggish reaction kinetics usually result in low efficiency. Herein, we designed kind quaternary PdCuCoZn medium-entropy alloy (MEA) metallene for highly selective electrosynthesis. The random occupation Cu, Co, Zn with lower electronegativity face-centered cubic lattice Pd-based enables abundant electron donation from transition metals adjacent Pd atoms, leading formation charge-polarized Pdδ--Cu/Co/Znδ+ sites. Considering that pivotal C- N-intermediates, namely, *CO *NH2, are electrophilic nucleophilic, respectively, such strong charge polarization would greatly benefit their respective stabilization. stable adsorption bonded electron-rich sites *NH2 electron-deficient Cu/Co/Zn-based demonstrated by combination situ characterizations theoretical calculations. proof-of-concept MEA achieves maximum yield rate 1840 μg h-1 mg-1 high Faradaic efficiency 70.2%, surpassing most reported state-of-the-arts. Our strategy proposed this work believed enlighten design an effective catalyst used multistep reactions.

Язык: Английский

Процитировано

0
Maximizing Available Active Hydrogen on FeNi Substitutional Solid-Solution Alloy to Boost Electrosynthesis of Ammonia from Nitrate DOI
Xing Sun, Yanzheng He, Mengfan Wang

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Фев. 20, 2025

Electrochemical nitrate reduction reaction (NO3RR) stands out as a promising route for sustainable ammonia synthesis, in which active hydrogen (*H) plays crucial role both the deoxygenation and hydrogenation steps. However, regulation of surface *H is still overlooked, without intervention, competing evolution kinetically more favored over NO3RR, leaving current system far from satisfactory. Herein, based on reverse utilization Sabatier principle, series FexNiy substitutional solid-solution alloys (SSAs) are synthesized to manipulate behavior enhanced NO3RR. Upon precise optimization alloy composition, d-band center HER-active Ni shifts toward Fermi level, endowing catalyst with strong interaction greatly prolonging its lifetime, enables abundant supply facilitate As expected, maximum NH3 yield rate 31.46 mmol h-1 mg-1 delivered optimized Fe3Ni1-SSA, considerably higher than most extensively reported works. Several situ characterizations combined gain in-depth insight. Especially, Fourier transform infrared spectroscopy internal reflection mode directly observes enrichment surface, while accompanied facilitation NO3RR process verified by external mode.

Язык: Английский

Процитировано

0
High-efficiency interfacial solar steam generation by metallophthalocyanine COFs coated on hydrogels DOI

Xu Lu,

Xiaoyang Fang,

Yucheng Jin

и другие.

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161018 - 161018

Опубликована: Фев. 1, 2025

Язык: Английский

Процитировано

0
Construction of MOF-on-MOF-derived composites with coexisting octahedrons and dodecahedrons for superior photocatalytic nitrogen fixation DOI

Runxian Hao,

Zaihang Zheng,

Yixin Li

и другие.

Journal of Catalysis, Год журнала: 2025, Номер unknown, С. 116121 - 116121

Опубликована: Апрель 1, 2025

Язык: Английский

Процитировано

0
Thiadiazole/Triazole-based covalent organic frameworks for efficient photocatalytic reduction of U(VI): Isomeric effect and delocalization degree DOI
Xin Zhong, Ji Zhang, Jing Xu

и другие.

Separation and Purification Technology, Год журнала: 2025, Номер 367, С. 132890 - 132890

Опубликована: Апрель 8, 2025

Язык: Английский

Процитировано

0
Multivariate covalent organic frameworks with tailored electrostatic potential promote nitrate electroreduction to ammonia in acid DOI Creative Commons

Qiyang Cheng,

Sisi Liu, Yanzheng He

и другие.

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Апрель 19, 2025

The direct synthesis of ammonia from nitrate (NO3-) reduction in acid is a promising approach for industrialization. However, the difficulty arises intense competition with inevitable hydrogen evolution reaction, which favoured due to overwhelming protons (H+). Here, we systematically explore and rationally optimize microenvironment using multivariate covalent organic frameworks (COFs) as catalyst adlayers promote nitrate-to-ammonia conversion acid. With application tailored positive electrostatic potential generated over COFs, both mass transfer NO3- H+ are regulated via appropriate interactions, thus realizing priority NO3RR respect HER or NO3--to-NO2-. As result, an NH3 yield rate 11.01 mmol h-1 mg-1 corresponding Faradaic efficiency 91.0% attained, solid NH4Cl high purity 96.2% directly collected acid; therefore, this method provides practical economically valorising wastewater into valuable ammonia.

Язык: Английский

Процитировано

0
Emerging electrocatalysts for green ammonia production: Recent progress and future outlook DOI Creative Commons
Sajid Mahmood, Shahid Iqbal,

Zeping Wang

и другие.

Arabian Journal of Chemistry, Год журнала: 2024, Номер 17(10), С. 105950 - 105950

Опубликована: Авг. 7, 2024

In the Haber-Bosch process (HBp), which uses elevated pressure and temperature to produce more concentration of nitrogen hydrogen gases, 90% 175 million metric tons NH3 generated worldwide in 2016 were manufactured this process. According road plan for sustainable ammonia production sustainably, using water as a reducing agent is most effective way fix close-quarters ambiance. A complete explanation theoretical practical work on electrocatalytic reduction provided article, with special attention paid low selectivity comparison protons hydrogen. Since they are essential accurately achieving high Faradaic efficiency (FE), their information outlines electrocatalysts, electrolyte selection criteria, managed experiment design. Under diverse conditions, evolution theory examined. Finally, feedback given field's present issues prospects.

Язык: Английский

Процитировано

2
Double enhancement of protonation and conjugation in donor–imine–donor covalent organic frameworks for photocatalytic hydrogen evolution DOI Creative Commons
Huan He,

Rongchen Shen,

Y. H. Yan

и другие.

Chemical Science, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

Three donor–imine–donor COFs as relatively pure model materials were utilized to reveal that protonation and conjugation can enhance exciton dissociation, light absorption electron transport, thus achieving a remarkable H 2 evolution rate.

Язык: Английский

Процитировано

1
Impact of Interfaces on the Performance of Covalent Organic Frameworks for Photocatalytic Hydrogen Production DOI Open Access
Lin Wang, Yong Zhang

Small, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 18, 2024

The rise in global temperatures and environmental contamination resulting from traditional fossil fuel usage has prompted a search for alternative energy sources. Utilizing solar to drive the direct splitting of water hydrogen production emerged as promising solution these challenges. Covalent organic frameworks (COFs) are ordered, crystalline materials made up molecules linked by covalent bonds, featuring permanent porosity wide range structural topologies. COFs serve suitable platforms solar-driven produce hydrogen, their building blocks can be tailored possess adjustable band gaps, charge separation capabilities, porosity, wettability, chemical stability. Here, impact interface context photocatalytic reaction is focused propose strategies enhance performance photocatalysis. In particular, how hybrid interfaces affect focused.

Язык: Английский

Процитировано

1
Fe─S Bond‐Mediated Efficient Electron Transfer in Quantum Dots/Metal‐Organic Frameworks for Boosting Photoelectrocatalytic Nitrogen Fixation DOI

Yuman Jiang,

Fengying Zhang,

Yanglin Mei

и другие.

Small, Год журнала: 2024, Номер unknown

Опубликована: Сен. 5, 2024

Abstract Effective electron supply to produce ammonia in photoelectrochemical nitrogen reduction reaction (PEC NRR) remains challenging due the sluggish multiple proton‐coupled transfer and unfavorable carrier recombination. Herein, InP quantum dots decorated with sulfur ligands (InP QDs‐S 2− ) bound MIL‐100(Fe) as a benchmark catalyst for PEC NRR is reported. It found that can combined via Fe─S bonds bridge facilitate by experimental results. The formation of from inorganic S QDs Fe metal sites within 52 ps, ensuring more efficient electron‐hole separation confirmed time‐resolved spectroscopy. More importantly, process photo‐induced be traced situ attenuated total reflection surface‐enhanced infrared tests, certifying effective promote N≡N dissociation N 2 hydrogenation. As result, /MIL‐100(Fe) exhibits prominent performance an outstanding NH 3 yield 0.58 µmol cm −2 h −1 (3.09 times higher than MIL‐100(Fe)). This work reveals important ultrafast dynamic mechanism modified metal‐organic frameworks, providing new guideline rational design MOFs photocathodes.

Язык: Английский

Процитировано

0