Rational electrocatalyst design for selective nitrate reduction to ammonia DOI Open Access
Zhaodong Niu, Guoxiong Wang

Chemical Physics Reviews, Journal Year: 2025, Volume and Issue: 6(1)

Published: Feb. 26, 2025

The electrocatalytic nitrate (NO3−) reduction reaction (NO3RR) is an attractive strategy for sustainable ammonia (NH3) synthesis, contributing to the artificial nitrogen cycle and renewable energy storage. However, selective conversion of NO3− NH3 remains challenging due complex multi-electron transfer processes, which result in numerous by-products, low yield rate, Faradaic efficiency. Additionally, electrochemical sensitivity catalyst structure complicates identifying active sites. Herein, we introduce mechanisms situ characterization technologies NO3RR production. Then, a summary theoretical research advances guide design catalyst, including density functional theory calculations, activity descriptors, machine learning. Furthermore, discuss strategies optimize performance NO3RR, focusing on nitrogenous-intermediate adsorption, proton tandem catalysis. Finally, challenges opportunities highly efficient are summarized.

Language: Английский

Advanced electrocatalysts with unusual active sites for electrochemical water splitting DOI Creative Commons
Hainan Sun, Xiaomin Xu, Hyunseung Kim

et al.

InfoMat, Journal Year: 2023, Volume and Issue: 6(1)

Published: Nov. 27, 2023

Abstract Electrochemical water splitting represents a promising technology for green hydrogen production. To design advanced electrocatalysts, it is crucial to identify their active sites and interpret the relationship between structures performance. Materials extensively studied as electrocatalysts include noble‐metal‐based (e.g., Ru, Ir, Pt) non‐noble‐metal‐based 3d transition metals) compounds. Recently, advancements in characterization techniques theoretical calculations have revealed novel unusual sites. The present review highlights latest achievements discovery identification of various unconventional electrochemical splitting, with focus on state‐of‐the‐art strategies determining true establishing structure–activity relationships. Furthermore, we discuss remaining challenges future perspectives development next‐generation By presenting fresh perspective reaction involved this aims provide valuable guidance study industrial applications. image

Language: Английский

Citations

95
Tandem Nitrate‐to‐Ammonia Conversion on Atomically Precise Silver Nanocluster/MXene Electrocatalyst DOI
Lin Liu, Sujun Zheng, Hong Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(8)

Published: Jan. 5, 2024

Abstract Electrocatalytic reduction of nitrate (NO 3 RR) to synthesize ammonia (NH ) provides a competitive manner for carbon neutrality and decentralized NH synthesis. Atomically precise nanoclusters, as an advantageous platform investigating the NO RR mechanisms actual active sites, remain largely underexplored due poor stability. Herein, we report 4 9 [Ag (mba) ] nanoclusters (Ag NCs) loaded on Ti C 2 MXene /MXene) highly efficient performance towards ambient synthesis with improved stability in neutral medium. The composite structure Ag NCs enables tandem catalysis process reduction, significantly increasing selectivity FE . Besides, compared individual NCs, /MXene has better current density performed no decay after 108 hours reaction. This work strategy improving catalytic activity atomically metal expanding mechanism research application NCs.

Language: Английский

Citations

59
Ambient Electrochemical Ammonia Synthesis: From Theoretical Guidance to Catalyst Design DOI Creative Commons

Jianjia Mu,

Xuan‐Wen Gao,

Tong Yu

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(15)

Published: Feb. 12, 2024

Abstract Ammonia, a vital component in the synthesis of fertilizers, plastics, and explosives, is traditionally produced via energy‐intensive environmentally detrimental Haber–Bosch process. Given its considerable energy consumption significant greenhouse gas emissions, there growing shift toward electrocatalytic ammonia as an eco‐friendly alternative. However, developing efficient electrocatalysts capable achieving high selectivity, Faraday efficiency, yield under ambient conditions remains challenge. This review delves into decades‐long research synthesis, highlighting evolution fundamental principles, theoretical descriptors, reaction mechanisms. An in‐depth analysis nitrogen reduction (NRR) nitrate (NitRR) provided, with focus on their electrocatalysts. Additionally, theories behind electrocatalyst design for are examined, including Gibbs free approach, Sabatier principle, d ‐band center theory, orbital spin states. The culminates comprehensive overview current challenges prospective future directions development NRR NitRR, paving way more sustainable methods production.

Language: Английский

Citations

32
A Coherent Pd–Pd16B3 Core–Shell Electrocatalyst for Controlled Hydrogenation in Nitrogen Reduction Reaction DOI

Yankun Wen,

Tongde Wang,

Jiace Hao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(34)

Published: March 7, 2024

Abstract The manipulation of surface catalytic sites has rarely been explored for metal borides, and the subsurface effects on electrocatalytic activity nitrogen reduction reaction (NRR) remain unknown. Herein, this work develops a core–shell nanoparticle catalyst with Pd core that ensures high electron transfer rates an 16 B 3 atomical shell possess tunable active regulating NRR. atomic structural evolution from to is investigated by precisely controlling atom diffusion, molecular rearrangement, d – sp orbital hybridization. Pd/Pd nanocrystals exhibit exceptional NRR performance NH Faradaic efficiency 30.8%, which superior those pristine (1.2%) B‐doped (4.8%) under identical conditions, yield rate 0.81 µmol h −1 cm −2 . This discovers could promote selectivity separating hydrogen proceeded hole bridge sites, provide excellent conductivity through regulated interactions. Consequently, controlled chemical ordering palladium boride surfaces provides insight into synthesis advanced electrocatalysts.

Language: Английский

Citations

21
Recent Progress and Perspectives on Transition Metal-Based Electrocatalysts for Efficient Nitrate Reduction DOI
Jun Zhou,

Sanshuang Gao,

Guangzhi Hu

et al.

Energy & Fuels, Journal Year: 2024, Volume and Issue: 38(8), P. 6701 - 6722

Published: April 8, 2024

Electrochemical nitrate reduction is the process of converting into ammonia or nitrogen using electric energy. This saves energy, protects environment, and an important technology for resource recovery water purification. paper examines recent advances in electrochemical research analyzes reaction mechanism path as well influence various factors on through thermodynamic kinetic principles. Second, catalytic performances transition metal electrocatalysts form single metals, alloys, oxides, composites are analyzed detail, which lays foundation rational development new, efficient, stable electrocatalysts. Finally, future directions prospects envisioned.

Language: Английский

Citations

20
Nitrogenous Intermediates in NOx‐involved Electrocatalytic Reactions DOI
Shunhan Jia, Limin Wu,

Hanle Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Jan. 16, 2024

Abstract Chemical manufacturing utilizing renewable sources and energy emerges as a promising path towards sustainability carbon neutrality. The electrocatalytic reactions involving nitrogen oxides (NO x ) offered potential strategy for synthesizing various nitrogenous chemicals. However, it is currently hindered by low selectivity/efficiency limited reaction pathways, mainly due to the difficulties in controllable generation utilization of intermediates. In this minireview, focusing on intermediates NO ‐involved reactions, we discuss newly developed methodologies studying controlling generation, conversion, intermediates, which enable recent developments that yield products, including ammonia (NH 3 ), organonitrogen molecules, compounds exhibiting unconventional oxidation states. Furthermore, also make an outlook highlight future directions emerging field reactions.

Language: Английский

Citations

19
Hollow Square Ni-Doped Copper Oxide Catalyst Boosting Electrocatalytic Nitrate Reduction DOI
Yi Li, Jinshan Wei,

Hexing Lin

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1672 - 1683

Published: Jan. 16, 2025

The electrochemical nitrate reduction reaction to ammonia (NRA) is gaining increasing attention as an eco-friendly approach convert harmful pollutants into high-value product ammonia. NRA involves two critical rate-determining steps: hydrogenation of the *NO and *NOH intermediates. composite Ni Cu has been demonstrated exhibit synergistic catalytic effects; however, research on combination CuO remains limited. Herein, advanced Ni-doped copper oxide catalyst with a hollow square morphology (Ni–CuO) reported Faradaic efficiency 95.26% at −0.8 V vs RHE high yield rate 0.94 mmol h–1 cm–2, demonstrating selectivity stability. Complementary analyses that active hydrogen generated sites facilitates *NOx adsorbed sites. Theoretical computations further confirm thermodynamic viability this bimetallic mechanism. Furthermore, Al–NO3– battery open-circuit voltage was constructed by using Ni–CuO cathode. This work presents synergistically modulated for complex processes introduces highly efficient capable simultaneous NH3 synthesis electrical energy conversion, underscoring its potential in catalysis development chemical industries.

Language: Английский

Citations

4
Carbon dots-boosted active hydrogen for efficient electrocatalytic reduction of nitrate to ammonia DOI
Dongxu Zhang, Yanhong Liu, Di Li

et al.

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: unknown, P. 178694 - 178694

Published: Jan. 1, 2025

Language: Английский

Citations

2
Accelerating proton coupled electron transfer by confined Cu-Ni bimetallic clusters for boosting electrochemical hydrodeoxygenation of nitrate DOI
Jiayi Zhang, Lu Liu, Nan Hu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125195 - 125195

Published: Feb. 1, 2025

Language: Английский

Citations

2
Transition Metal Single‐Atom Catalysts for the Electrocatalytic Nitrate Reduction: Mechanism, Synthesis, Characterization, Application, and Prospects DOI

Tianyi Xiang,

Yuntao Liang,

Yuxi Zeng

et al.

Small, Journal Year: 2023, Volume and Issue: 19(41)

Published: June 9, 2023

Excessive accumulation of nitrate in the environment will affect human health. To combat pollution, chemical, biological, and physical technologies have been developed recently. The researcher favors electrocatalytic reduction reaction (NO3 RR) because low post-treatment cost simple treatment conditions. Single-atom catalysts (SACs) offer great activity, exceptional selectivity, enhanced stability field NO3 RR their high atomic usage distinctive structural characteristics. Recently, efficient transition metal-based SACs (TM-SACs) emerged as promising candidates for RR. However, real active sites TM-SACs applied to key factors controlling catalytic performance process remain ambiguous. Further understanding mechanism is practical significance exploring design stable SACs. In this review, from experimental theoretical studies, mechanism, rate-determining steps, essential variables affecting activity selectivity are examined. terms RR, characterization, synthesis then discussed. order promote comprehend on TM-SACs, finally highlighted, together with current problems, remedies, way forward.

Language: Английский

Citations

38