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

и другие.

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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.

Язык: Английский

Promoting Electroreduction of CO2 and NO3− to Urea via Tandem Catalysis of Zn Single Atoms and In2O3‐x DOI
Ying Zhang, Zhuohang Li, Kai Chen

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of CO 2 and NO 3 − (UECN) offers an innovative route for converting waste /NO into valuable urea. Herein, Zn single atoms anchored on oxygen vacancy (OV)‐rich In O 3‐x (Zn 1 /In ) are developed as a highly active selective UECN catalyst, delivering the highest urea yield rate 41.6 mmol h −1 g urea‐Faradaic efficiency 55.8% at −0.7 V in flow cell, superior to most previously reported catalysts. situ spectroscopic measurements theoretical calculations unveil synergy In/Zn sites OVs promoting process via tandem catalysis mechanism, where ‐OV site activates form * NH while In‐OV CO. The formed spontaneously migrates nearby then couples with generate CONH which is ultimately converted

Язык: Английский

Процитировано

43
Promoting active hydrogen supply for kinetically matched tandem electrocatalytic nitrate reduction to ammonia DOI
Biyu Kang, Bincheng Xu, Zhixuan Chen

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 360, С. 124528 - 124528

Опубликована: Авг. 24, 2024

Язык: Английский

Процитировано

26
CoNiOOH nanosheets array enables highly effective value-added chemicals production via nitrite and sulfide electrolysis DOI
Miaosen Yang, Tianran Wei,

Chunhui Zeng

и другие.

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 155799 - 155799

Опубликована: Сен. 1, 2024

Язык: Английский

Процитировано

20
Synergistic Cu Single Atoms and MoS2‐Edges for Tandem Electrocatalytic Reduction of NO3− and CO2 to Urea DOI

Wenyu Du,

Zeyi Sun,

Kai Chen

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(43)

Опубликована: Авг. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) under ambient conditions is recognized as an appealing approach for effective sustainable urea production, while it requires high‐efficiency UENC electrocatalysts to promote the C─N coupling hydrogenation processes. Herein, single‐atom Cu anchored on MoS (Cu 1 ‐MoS ) explored a highly active selective catalyst. Theoretical calculations operando spectroscopic characterizations unveil synergistic tandem catalysis UENC, where single atoms trigger early coupling, ‐edges key step * NH COOHNH generation. Strikingly, equipped in flow cell achieves excellent performance with maximum urea‐Faradaic efficiency 57.02% at −0.6 V corresponding yield rate 23.3 mmol h −1 g , surpassing nearly all previously reported catalysts.

Язык: Английский

Процитировано

19
Magneto‐Electrochemical Ammonia Synthesis: Boosting Nitrite Reduction Activity by the Optimized Magnetic Field Induced Spin Polarized System DOI
Ashadul Adalder, Koushik Mitra,

Narad Barman

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(42)

Опубликована: Сен. 25, 2024

Abstract Using low and optimized magnetic field along with electric is a novel strategy to facilitate electrochemical nitrite reduction reaction (NO 2 RR). Herein, the assisted electrocatalytic ammonia synthesis employing spin‐thrusted β‐MnPc at 95 mT explored. The calculated rate of generation 16603.4 µg h −1 mg cat , which almost twice that nonpolarized manganese phthalocyanine (MnPc) catalyst. Additionally, Faradaic efficiency (FE) –0.9 V versus RHE found be 92.9%, significantly higher compared MnPc In presence external field, catalysts provide better electron transfer channel results in lower charge resistance hence performances. Density functional theory (DFT) result further verifies induced has potential barrier (0.51 eV) for protonation NO* than (1.08 eV), confirms enhanced ammonia.

Язык: Английский

Процитировано

19
Atomically Dispersed Cu on In2O3 for Relay Electrocatalytic Conversion of Nitrate and CO2 to Urea DOI
Ying Zhang, Zhuohang Li,

Chaofan Qiang

и другие.

ACS Nano, Год журнала: 2024, Номер 18(36), С. 25316 - 25324

Опубликована: Авг. 26, 2024

Urea electrosynthesis from coelectrolysis of NO

Язык: Английский

Процитировано

18
Tandem Active Sites in Cu/Mo‐WO3 Electrocatalysts for Efficient Electrocatalytic Nitrate Reduction to Ammonia DOI Creative Commons
Ying Dai, Shuangjun Li, Xue Li

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract Electrocatalytic NO 3 − reduction to NH is a promising technique for both ammonia synthesis and nitrate wastewater treatment. However, this conversion involves tandem processes of H 2 O dissociation hydrogenation, leading inferior Faraday efficiency (FE) yield rate. Herein, catalyst by anchoring atomically dispersed Cu species on Mo‐doped WO (Cu 5 /Mo 0.6 ‐WO ) the RR constructed, which achieves superior FE N 98.6% rate 26.25 mg h −1 cat at −0.7 V (vs RHE) in alkaline media, greatly exceeding performance Mo /WO counterparts. Systematic electrochemical measurement results reveal that promoted activation sites, accompanying accelerated water producing active hydrogens are responsible performance. In situ infrared spectroscopy theoretical calculation further demonstrate sites accelerate , dopant activates adjacent resulting decreased energy barrier * stepwise hydrogenation processes, making thermodynamically favorable. This work demonstrates critical role atomic level enhancing electrocatalytic paving feasible avenue developing high‐performance electrocatalysts.

Язык: Английский

Процитировано

5
A Copper–Zinc Cyanamide Solid-Solution Catalyst with Tailored Surface Electrostatic Potentials Promotes Asymmetric N-Intermediate Adsorption in Nitrite Electroreduction DOI Creative Commons

Jiacheng Jayden Wang,

Huong Thi Bui,

Xunlu Wang

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер 147(9), С. 8012 - 8023

Опубликована: Фев. 18, 2025

The electrocatalytic nitrite reduction (NO2RR) converts nitrogen-containing pollutants to high-value ammonia (NH3) under ambient conditions. However, its multiple intermediates and multielectron coupled proton transfer process lead low activity NH3 selectivity for the existing electrocatalysts. Herein, we synthesize a solid-solution copper-zinc cyanamide (Cu0.8Zn0.2NCN) with localized structure distortion tailored surface electrostatic potential, allowing asymmetric binding of NO2-. It exhibits outstanding NO2RR performance Faradaic efficiency ∼100% an yield 22 mg h-1 cm-2, among best such process. Theoretical calculations in situ spectroscopic measurements demonstrate that Cu-Zn sites coordinated linear polarized [NCN]2- could transform symmetric [Cu-O-N-O-Cu] CuNCN-NO2- [Cu-N-O-Zn] configuration Cu0.8Zn0.2NCN-NO2-, thus enhancing adsorption bond cleavage. A paired electro-refinery Cu0.8Zn0.2NCN cathode reaches 2000 mA cm-2 at 2.36 V remains fully operational industrial-level 400 >140 h production rate ∼30 mgNH3 cm-2. Our work opens new avenue tailoring potentials using strategy advanced electrocatalysis.

Язык: Английский

Процитировано

3
Electrocatalytic Urea Production with Nitrate and CO2 on a Ru‐Dispersed Co Catalyst DOI Open Access

Yuying Wan,

Zhuoyan Zhang,

Xiaomei Wang

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 12, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) provides an alternative route for realizing efficient sustainable urea production. In this work, single‐atom Ru dispersed on Co (Ru 1 Co) is demonstrated as effective robust catalyst the UENC. situ spectroscopic measurements theoretical simulations unravel cooperative effect sites to promote UENC process via a tandem catalysis mechanism, where site activates adsorption hydrogenation form * NH , while hydrogenation/deoxygenation CO. The generated then transferred nearby which promotes C─N coupling toward formation. Strikingly, assembled in flow cell shows highest urea‐Faradaic efficiency 50.1% with corresponding yield rate 22.34 mmol h −1 g at −0.5 V (RHE), superior most reported catalysts

Язык: Английский

Процитировано

16
Single-Atom Rh1 Alloyed Co for Urea Electrosynthesis from CO2 and NO3– DOI

Yuying Wan,

Zhuoyan Zhang,

Jinmei Qian

и другие.

Nano Letters, Год журнала: 2024, Номер 24(35), С. 10928 - 10935

Опубликована: Авг. 20, 2024

Single-atom Rh

Язык: Английский

Процитировано

10