Enabling Unconventional “Alternating‐Distal” N2 Reduction Pathway for Efficient Ammonia Electrosynthesis DOI Open Access
Chu Zhang, Qing Wang, Zeyu Li

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

Abstract The general understanding on the reaction path is that electrocatalytic N 2 reduction follows either individual associative alternating or distal pathways, where efficient activation and selective NH 3 production are very challenging. Herein, an unconventional “alternating‐distal” pathway was achieved by shifting “*NHNH →*NH ” to + step boost synthesis with amorphous CeMnO x electrocatalyst. In this process, realized through π back donation Mn site, while Mn/Ce dual active sites could regulate intermediate configurations avoid nitrogen‐containing by‐product formation. Such affirmed in situ spectroscopic analyses theoretical calculations. a neutral media, average ammonia rate of 82.8 µg h −1 mg outstanding Faradaic efficiency 37.3% were attained. This work validated mechanism synthesis, which might be extended other catalytic process multiple possible paths.

Language: Английский

The Electron‐Rich Interface Regulated MBene by S‐Bridge Guided to Enhance Nitrogen Fixation under Environmental Conditions DOI Open Access

Kun Cheng,

Shaobin Li,

Qingyu Cheng

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 15, 2024

Abstract The underutilization of active sites limits the performance enhancement 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo on surface MBene is successfully constructed by using an site electron optimization strategy, which increases charge density around enhances activation ability catalyst to N 2 molecules. It noteworthy that FeS ‐MBene demonstrates low intrinsic potential for (−0.2 V vs RHE). more favorable adsorption comparison hydrogen atoms, thereby it can effectively inhibit evolution (HER). Under −0.2 versus RHE, ammonia yield rate 37.13 ± 1.31 µg h −1 mg , FE 55.97 2.63%. Density functional theory (DFT) calculations demonstrate serves as . formation heterostructure transfer, resulting becoming electron‐rich state favor subsequent hydrogenation steps. This work offers significant insights into design utilization MBene‐based catalysts NRR.

Language: Английский

Citations

17
Pumping Electrons from Oxygen-Bridged Cobalt for Low-Charging-Voltage Zn-Air Batteries DOI

Yuchao Wang,

Q. X. Li, Meng Wang

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(43), P. 13653 - 13661

Published: Oct. 21, 2024

Reducing the charging voltage is a prerequisite for improving chargeability and energy efficiency of Zn-air batteries (ZABs). Herein, Fe

Language: Английский

Citations

16
Precious-Metal-Free Mo-MXene Catalyst Enabling Facile Ammonia Synthesis Via Dual Sites Bridged by H-Spillover DOI Creative Commons

Yanliang Zhou,

Lili Liang,

Congying Wang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(33), P. 23054 - 23066

Published: Aug. 12, 2024

To date, NH3 synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due inverse relationship between N2 dissociation barrier and NHx (x = 1–3) desorption energy. Herein, we demonstrate NPM (Co, Ni, Re)-mediated Mo2CTx MXene (where Tx denotes OH group) achieve efficient conditions. In particular, rate over Re/Mo2CTx Ni/Mo2CTx can reach 22.4 21.5 mmol g–1 h–1 at 400 °C 1 MPa, respectively, higher than that NPM-based Cs–Ru/MgO ever reported. Experimental theoretical studies reveal Mo4+ has a strong ability for activation; thus, rate-determining step shifted from conventional NH2* formation. mainly responsible H2 activation, high reactivity spillover hydrogen electron transfer N-rich surface efficiently facilitate nitrogen hydrogenation subsequent NH3. With synergistic effect dual active sites bridged by H-spillover, NPM-mediated circumvent major obstacle, making efficient.

Language: Английский

Citations

13
Highly crystalline benzothiadiazole covalent organic framework for enhanced Cr(VI) photocatalytic reduction by constructing donor-acceptor structure DOI
Chen Wang, Wen Lu, Wenhui Song

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 361, P. 124583 - 124583

Published: Sept. 8, 2024

Language: Английский

Citations

10
Axial Chlorine-Induced Symmetry-Breaking Iron Single-Atom Catalyst for Electrochemical Ammonia Synthesis DOI

Jieying Wan,

Ji Yang,

Na Yang

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 4507 - 4518

Published: March 3, 2025

Language: Английский

Citations

2
Main‐Group Metal‐Nonmetal Dynamic Proton Bridges Enhance Ammonia Electrosynthesis DOI
Yuntong Sun, Liming Dai, Kai Dong

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(45)

Published: Aug. 13, 2024

The electrochemical nitrogen reduction reaction (eNRR) is a crucial process for the sustainable production of ammonia (NH

Language: Английский

Citations

9
Identifying Highly Active and Selective Cobalt X‐Ides for Electrocatalytic Hydrogenation of Quinoline DOI Open Access

Han Du,

Tianyi Wang, Meng Li

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Sept. 2, 2024

Abstract Earth‐abundant Co X‐ides are emerging as promising catalysts for the electrocatalytic hydrogenation of quinoline (ECHQ), yet challenging due to limited fundamental understanding ECHQ mechanism on X‐ides. This work identifies catalytic performance differences in and provides significant insights into ECHQ. Among selected X‐ides, 3 O 4 presents best with a high conversion 98.2% 100% selectivity at ambient conditions. The sites present higher proportion 2‐coordinated hydrogen‐bonded water interface than other low negative potential, which enhances kinetics subsequent dissociation produce H*. An ideal 1,4/2,3‐H* addition pathway surface spontaneous desorption 1,2,3,4‐tetrahydroquinoline is demonstrated through operando tracing theoretical calculations. In comparison, 9 S 8 display lowest thermodynamic barrier H* formation step, suppresses hydrogenation; while Co(OH)F CoP undergo 1,2,3,4‐ 4,3/1,2‐H* respectively barriers thus quinoline. Moreover, wide substrate scope allows excellent derivatives N ‐heterocyclic substrates.

Language: Английский

Citations

9
Vacancy engineering of BiFeO3 perovskite for low-barrier electrochemical nitrogen fixation DOI

Jianli Nan,

Youxing Fang, Kai Rong

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 357, P. 124328 - 124328

Published: June 24, 2024

Language: Английский

Citations

7
Transition Metal‐Gallium Intermetallic Compounds with Tailored Active Site Configurations for Electrochemical Ammonia Synthesis DOI Creative Commons

Huaifang Zhang,

Chaoqun Ma,

Yichi Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(49)

Published: Sept. 4, 2024

Abstract Gallium (Ga) with a low melting point can serve as unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy transition metal‐Ga IMCs endows them high catalytic stability. Meanwhile, their tunable crystal structures offer possibility to tailor configurations active sites meet requirements for specific applications. Herein, we present general method preparing range IMCs, including Co−Ga, Ni−Ga, Pt−Ga, Pd−Ga, and Rh−Ga IMCs. structurally ordered CoGa body‐centered cubic ( bcc ) structure are uniformly dispersed on nitrogen‐doped reduced graphene oxide substrate (O‐CoGa/NG) deliver outstanding nitrate reduction reaction (NO 3 RR) performance, making excellent catalysts construct highly efficient rechargeable Zn‐NO − battery. Operando studies theoretical simulations demonstrate that electron‐rich environments around Co atoms enhance adsorption strength *NO intermediate simultaneously suppress hydrogen, thus improving NO RR activity selectivity.

Language: Английский

Citations

7
Comprehensive Insight Into Electronic Modulation of Rare‐Earth Elements for Enhancing Electrocatalytic Performance of Atomically Dispersed Materials DOI Open Access
Yanhui Cao, Xuerong Zheng, Yida Deng

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 2, 2025

Abstract Atomically dispersed materials have been a thriving research field due to their maximum atomic utilization and remarkable performance in energy conversion storage systems. Owing the large radius, strong oxophilicity, unique electronic properties, rare‐earth (RE) elements widely investigated as oxide carriers promoters atomically manipulate regulate structure of active species. Single‐atom state with an adjustable coordination environment on N‐doped carbon endows RE metals special states outstanding catalytic performances. A thorough comprehension modulation mechanism paves way for construction advanced RE‐based electrocatalysts high activity, stability, selectivity. This review provides widespread insight into roles modulating properties combined structure–performance relationship electrocatalysis processes. The characteristic physical chemical are highlighted, synthetic strategy is discussed. Finally, summary perspectives rational design development highly efficient catalysts proposed. aims provide guideline promoting effective functional materials.

Language: Английский

Citations

1