Modifying Microenvironment in Van der Waals Gap by Cu/N Co‐Doping Strategy for Highly Efficient Nitrite Reduction to Ammonia DOI Creative Commons

Heen Li,

Yuanzhe Wang,

Kuo Wei

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 24, 2025

Abstract Electroreduction of nitrite to ammonia has significant promise for economical NH 3 electrosynthesis and wastewater treatment. Herein, sulfur vacancies rich Cu─N co‐doped SnS 2 nanosheet is designed as a highly active durable NO RR catalyst. Benefiting from the strategy, Cu/N‐SnS 2‐x achieves highest yield rate 18.15mg h −1 mg cat at −0.935 V (vs RHE) excellent Faradaic Efficiency 95.73% −0.835 RHE). In situ FT‐IR in XPS proves that greater capacity atomic hydrogen generation, which facilitates conversion maintains structural stability during process. Theoretical calculations reveal introduced effectively expose metal atoms inside make them adsorb efficiently, accelerates transformation ammonia. Besides, Cu N can form new electronic structure, induces an electron‐deficient state promotes adsorption reaction intermediates on Cu, reduces energy barrier reduction surface. The current exploration presents fresh prospects rational development effective electrocatalyst synthesizing nitrite.

Language: Английский

Synergistic Effect of Ni/Ni(OH)2 Core‐Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere‐Level Ammonia Production DOI

Xinyue Shi,

Minghui Xie,

Kaiwen Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Electrocatalytic reduction of nitrate to ammonia provides a green alternate the Haber-Bosch method, yet it suffers from sluggish kinetics and low yield rate. The follows tandem reaction nitrite subsequent hydrogenation generate ammonia, Faraday efficiency (FE) is limited by competitive hydrogen evolution reaction. Herein, we design heterostructure catalyst remedy above issues, which consists Ni nanosphere core Ni(OH)

Language: Английский

Citations

36
Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia DOI
Yuanbo Zhou, Lifang Zhang, Zebin Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Electrochemical reduction of nitrate to ammonia (NO

Language: Английский

Citations

34
Shear‐Strained Pd Single‐Atom Electrocatalysts for Nitrate Reduction to Ammonia DOI

Yunliang Liu,

Zechao Zhuang, Yixian Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 16, 2024

Electrochemical nitrate reduction method (NitRR) is a low-carbon, environmentally friendly, and efficient for synthesizing ammonia, which has received widespread attention in recent years. Copper-based catalysts have leading edge due to their good adsorption of *NO

Language: Английский

Citations

23
Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia DOI
Yuanbo Zhou, Lifang Zhang, Zebin Zhu

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(18)

Published: March 7, 2024

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) is a promising and eco‐friendly strategy for production. However, the sluggish kinetics eight‐electron transfer process poor mechanistic understanding strongly impedes its application. To unveil internal laws, herein, library Pd‐based bimetallene with various transition metal dopants (PdM (M=Fe, Co, Ni, Cu)) are screened learn their structure–activity relationship towards NO RR. The ultra‐thin structure metallene greatly facilitates exposure active sites, metals break electronic balance upshift d‐band center, thus optimizing intermediates adsorption. anisotropic characteristics these make RR activity in order PdCu>PdCo≈PdFe>PdNi>Pd, record‐high NH yield rate 295 mg h −1 cat along Faradaic efficiency 90.9 % achieved neutral electrolyte on PdCu bimetallene. Detailed studies further reveal that moderate N‐species (*NO *NO 2 ) adsorption ability, enhanced activation, reduced HER facilitate We believe our results will give systematic guidance future design catalysts.

Language: Английский

Citations

18
Co‐Catalytic Metal‐Support Interactions Design on Single‐Atom Alloy for Boosted Electro‐Reduction of Nitrate to Nitrogen DOI
Ziyang Wu, Xuxin Kang, Sen Wang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(45)

Published: May 28, 2024

Abstract The past decades have seen considerable imbalances in the nitrogen cycle due to excessive use of nitrate agriculture and industry. Electrocatalytic reduction (NO 3 RR) (N 2 ) holds significant potential for addressing pollution wastewater but suffers from nitrite formation sluggish hydrogeneration process. Here a single atom alloy (SAA) catalyst featuring atomically dispersed Ru on 2D Ni metal (Ru 1 Ni), proving remarkable performance − –N conversion (≈93%) N selectivity (≈99%)) through co‐catalytic metal‐support interactions (CMSI) effect is reported. Significantly, SAA achieves NO RR removal capacity as high 11.1 mg L −1 h cm −2 with 20 cycles stability (9 per cycle), surpassing most previously reported works. core boosting lies synergistically promoted activation accelerated hydrogenation oxide intermediates site substrate, respectively, revealed by various situ experiments theoretical simulations. DFT calculations indicate electron transfer substrate more robust interaction between Ru–Ni comparison that Ni–Ni. This work offers resilient methodology rational design highly efficient electrocatalysts CMSI modulation RR, illuminating arena treatment cycle.

Language: Английский

Citations

18
Regioselective Doping into Atomically Aligned Core–Shell Structures for Electrocatalytic Reduction of Nitrate to Ammonia DOI Open Access
Ying Zhang, Tianyi Gao, Fei Zhang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(46)

Published: Aug. 26, 2024

Abstract The electrochemical nitrate reduction reaction (NO 3 − RR) presents an environmentally friendly approach for efficient NO pollutant removal and ammonia (NH ) production, compared to the conventional Haber–Bosch approach. While core/shell engineering has demonstrated its potential in enhancing RR performance, significant synthetic challenges limited shell layer modification capabilities impede exploration of high‐performance catalysts. Herein, CuCoO/Co(OH) 2 structure via situ activation is synthesized. catalyst delivers a maximum NH Faradaic efficiency (FE) 94.7% at −0.5 V RHE with excellent durability selectivity over wide range potentials RR, surpassing electrocatalytic performance both undoped core components. outstanding Cu─CoO/Co(OH) ascribed enhanced charge transfer, stabilization key intermediates, regulation hydrogen adsorption Cu‐doped structure. Furthermore, assembled Zn−NO battery device attains peak current density exceeding 32 mA cm −2 yield up 145.4 µmol h −1 . work offers novel strategy sheds light on doping effects synthesis.

Language: Английский

Citations

13
Shear‐strained Pd Single‐atom Electrocatalysts for Nitrate Reduction to Ammonia DOI

Yunliang Liu,

Zechao Zhuang, Yixian Liu

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(43)

Published: July 16, 2024

Abstract Electrochemical nitrate reduction method (NitRR) is a low‐carbon, environmentally friendly, and efficient for synthesizing ammonia, which has received widespread attention in recent years. Copper‐based catalysts have leading edge due to their good adsorption of *NO 3 . However, the formation active hydrogen (*H) on Cu surfaces difficult insufficient, resulting large amount by‐product NO 2 − In this work, Pd single atoms suspended interlayer unsaturated bonds CuO formed dislocations (Pd−CuO) were prepared by low temperature treatment, located subjected shear stress dynamic effect support promote conversion into ammonia. The catalysis had an ammonia yield 4.2 mol. g cat −1 h , Faraday efficiency 90 % production at −0.5 V vs. RHE. situ characterization theoretical calculations indicate that effects carriers under obviously hydrogen, reduce reaction energy barrier decision‐making step further generation.

Language: Английский

Citations

12
Engineering Nickel Dopants in Atomically Thin Molybdenum Disulfide for Highly Efficient Nitrate Reduction to Ammonia DOI

Jiangnan Lv,

Xiaoting Sun, Fang Wang

et al.

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

Published: Sept. 16, 2024

Abstract The electrocatalytic nitrate reduction reaction (NO 3 − RR) presents a promising pathway for achieving both ammonia (NH ) electrosynthesis and water pollutant removal simultaneously. Among various electrocatalysts explored, 2D materials have emerged as candidates due to their ability regulate electronic states active sites through doping. However, the impact of doping effects in on mechanism NO RR remains relatively unexplored. Here, Ni‐doped MoS 2 (Ni‐MoS nanosheets are investigated model system, demonstrating enhanced performance compared undoped counterparts. By controlling concentration, Ni‐MoS achieve remarkable faradic efficiency (FE) 92.3% NH at −0.3 V RHE with excellent stability. mechanistic studies reveal that elevation performances originates from generation more hydrogen acceleration nitrite facilitated by Ni Combining experimental observations theoretical calculations it is revealed appropriate level can enhance *NO adsorption strength, thereby facilitating subsequent steps. Together demonstration Zn−NO battery devices, work provides new insights into design regulation material catalysts efficient RR.

Language: Английский

Citations

11
Synergistic rare-earth yttrium single atoms and copper phosphide nanoparticles for high-selectivity ammonia electrosynthesis DOI

Y. Cai,

Yanghua Li, Yi Xiao

et al.

Rare Metals, Journal Year: 2024, Volume and Issue: 43(11), P. 5792 - 5801

Published: June 18, 2024

Language: Английский

Citations

10
Copper–Nickel Oxide Nanosheets with Atomic Thickness for High‐Efficiency Sulfur Ion Electrooxidation Assisted Nitrate Electroreduction to Ammonia DOI
Xiaohui Wang,

Qing‐Ling Hong,

Liyang Shao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(48)

Published: Aug. 16, 2024

Abstract The nitrate electroreduction reaction (NO 3 RR) offers an eco‐friendly alternative to the Haber–Bosch technology for ammonia (NH ) synthesis. However, complex process and diverse products make efficient NH synthesis challenging. Therefore, rational design preparation of highly electrocatalysts are crucial NO RR. Herein, ultrathin copper‐nickel oxide (Cu‐NiO) nanosheets (Cu‐NiO UTNSs) synthesized via cyanogel‐NaBH 4 hydrolysis‐reduction method, which applied cathodic RR ‐assisted with anodic sulfur ion (S 2− oxidation (SOR) in electrolyzer. nanosheet structure, interaction between NiO Cu, formation oxygen vacancy contribute generating rich active sites, regulating electronic improving substance adsorption. Thus, Cu‐NiO UTNSs exhibit excellent electrocatalytic performance SOR. As a bifunctional UTNSs||Cu‐NiO electrolyzer, it can reach 10 mA cm −1 at only 0.1 V − ‐to‐NH conversion cathode S ‐to‐S 8 anode. This work provides promising approach producing value‐added chemicals low electrolysis voltage strategy pollutant treatment.

Language: Английский

Citations

10