Metal/covalent-organic framework-based electrocatalysts for electrochemical reduction of nitrate to ammonia DOI Creative Commons
Tarekegn Heliso Dolla, Boying Zhang, Thabo Matthews

и другие.

Coordination Chemistry Reviews, Год журнала: 2024, Номер 518, С. 216061 - 216061

Опубликована: Июль 8, 2024

The pervasive contamination of industrial, domestic, and agricultural wastewater with nitrate poses profound ecological public health risks. Traditional methods for remediating nitrate-laden water face formidable challenges due to its high solubility stability. However, a promising solution emerges in the form electrochemical reduction (eNO3RR), offering both efficient removal valuable ammonia generation sustainable manner. This review explores burgeoning field eNO3RR, focusing on recent advancements utilizing porous crystalline framework materials − metal–organic frameworks (MOFs) covalent-organic (COFs) as novel class electrocatalysts. These innovative exhibit unique properties such adjustable porosity, diverse structures, tunable pore sizes, well-defined active sites, making them ideal candidates enhancing efficiency selectivity under ambient conditions. By dissecting structure–activity relationship inherent MOF/COF-based electrocatalysts, this aims provide comprehensive understanding their role driving conversion NO3− NH3. Moreover, it identifies current proposes future prospects leveraging these advanced pollutants, glimpse into greener more effective approach remediation resource recovery.

Язык: Английский

Homogeneously Mixed Cu–Co Bimetallic Catalyst Derived from Hydroxy Double Salt for Industrial-Level High-Rate Nitrate-to-Ammonia Electrosynthesis DOI
Wonsik Jang, Dongrak Oh, Jin‐Young Lee

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(40), С. 27417 - 27428

Опубликована: Авг. 23, 2024

Electrocatalytic nitrate reduction reaction (NO

Язык: Английский

Процитировано

18
Enhanced Charge Carrier Dynamics on Sb2Se3 Photocathodes for Efficient Photoelectrochemical Nitrate Reduction to Ammonia DOI
Shijie Ren, Rui‐Ting Gao, Nhat Truong Nguyen

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(11)

Опубликована: Янв. 16, 2024

Abstract Ammonia (NH 3 ) is recognized as a transportable carrier for renewable energy fuels. Photoelectrochemical nitrate reduction reaction (PEC NO RR) offers sustainable solution nitrate‐rich wastewater treatment by directly converting solar to ammonia. In this study, we demonstrate the highly selective PEC ammonia production from RR constructing CoCu/TiO 2 /Sb Se photocathode. The constructed photocathode achieves an Faraday efficiency (FE) of 88.01 % at −0.2 V RHE and yield high 15.91 μmol h −1 cm −2 −0.3 with excellent onset potential 0.43 . Dynamics experiments theoretical calculations have demonstrated that possesses light absorption capacity, transfer capability, charge separation efficiencies. can effectively adsorb reactant − intermediate, CoCu co‐catalyst increases maximum Gibbs free difference between HER. Meanwhile, Co species enhances spin density Cu, states near Fermi level in pdos, which results activity on This work provides new avenue feasibility efficient synthesis wastewater.

Язык: Английский

Процитировано

17
Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia DOI
Yuanbo Zhou, Lifang Zhang, Zebin Zhu

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(18)

Опубликована: Март 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.

Язык: Английский

Процитировано

17
Efficient Electrochemical Nitrate Reduction to Ammonia Driven by a Few Nanometer-Confined Built-In Electric Field DOI
Maolin Zhang, Zedong Zhang, Shaolong Zhang

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10437 - 10446

Опубликована: Июнь 26, 2024

Converting nitrate (NO3–) to ammonia (NH3) through the electrochemical reduction method offers an appealing approach for wastewater treatment and facilitates nitrogen cycling in nature. However, this electrolytic involves a series of proton-coupled electron transfer processes comes with severe competing reactions. Consequently, there is significant demand catalysts exhibiting good catalytic activities selectivities. Here, copper–cobalt binary sulfide nanosheets varying Cu/Co compositions were prepared investigate synergy effects between components copper cobalt on their performance. As result, volcano-like correlation ratio electrocatalytic performance was built. The optimal catalyst CuxS–Co0.5 exhibited maximum Faradaic efficiency (FE) ∼95.6% at −1.4 V vs Ag/AgCl. highest yield rate 5.36 mg/h·cm2 achieved −1.6 Ag/AgCl, which 6.5- 3.8-fold relative those pure CuxS CoS2, respectively. By combining spectroscopy characterizations theoretical calculations, we revealed that built-in electric field confined few nanometers played critical role enhancing creating more active sites. Besides, its improved water dissociation capability essential hydrogenation intermediates, collectively contributing enhanced

Язык: Английский

Процитировано

17
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

17
Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst DOI

Yunliang Liu,

Zhiyu Zheng,

Sobia Jabeen

и другие.

Nano Research, Год журнала: 2024, Номер 17(6), С. 4889 - 4897

Опубликована: Фев. 8, 2024

Язык: Английский

Процитировано

16
Active Hydrogen for Electrochemical Ammonia Synthesis DOI Creative Commons
Guoqiang Gan, Hong Guo, Wenjun Zhang

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Апрель 15, 2024

Abstract Electrochemical ammonia synthesis (EAS) presents an attractive alternative to the Haber–Bosch process due benefits of energy saving, low carbon emission, environmental friendliness, and so on. However, competing hydrogen evolution reaction (HER) severely limits yield, selectivity, current efficiency NH 3 . Although accumulation self‐aggregation active (H*) are primary causes HER, it also serves as critical species intermediate for multistep hydrogenation deoxygenation processes. Therefore, sensible regulation H* generation consumption essential enhancing EAS performance. And is significant thoroughly review strategies control. Herein, a comprehensive introduction provide fundamental understanding its role in electrochemical reactions, including generation, conversion, identification, quantification protocols first proposed. In addition, control carefully summarized with particular focus on regulating enhance activity, Faradaic efficiency. Finally, remaining challenges perspectives discussed. This intended offer profound reactions development technology.

Язык: Английский

Процитировано

16
Carbon dots-boosted active hydrogen for efficient electrocatalytic reduction of nitrate to ammonia DOI
Dongxu Zhang, Yanhong Liu, Di Li

и другие.

Journal of Alloys and Compounds, Год журнала: 2025, Номер unknown, С. 178694 - 178694

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

2
Optimizing selectivity via steering dominant reaction mechanisms in steam reforming of methanol for hydrogen production DOI Creative Commons
Mengyuan Zhang, Zhi Liu, Yong Yan

и другие.

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

Опубликована: Фев. 24, 2025

Enhancing selectivity towards specific products remains a pivotal challenge in energy catalysis. Herein, we present strategy to refine via pathway optimization, exemplified by the rational design of catalysts for methanol steam reforming. Over traditional Pd/ZnO catalysts, direct decomposition key intermediates CH2O* into CO and H2 on PdZn alloys competes with oxidation CO2, leading inferior product distribution. To address this challenge, Cu is introduced modify catalytic dynamics, lowering dissociation barrier water provide more active hydroxyl groups CH2O*. Simultaneously, desorption PdCu elevated, thereby hindering decomposition. This dual functionality enhances both activity reforming reaction. By modulating activation patterns intermediate species, approach provides new insights catalyst improved reaction selectivity. Improving Here, authors introduce refining through

Язык: Английский

Процитировано

2
Periodic Adjacent Pd‐Fe Pair Sites for Enhanced Nitrate Electroreduction to Ammonia via Accelerating Proton Relay DOI
Meng Xie, Guihua Zhu, Haoyu Yang

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(33)

Опубликована: Май 29, 2024

Abstract Recently, bimetallic nanoparticles (NPs) are promising for driving nitrate (NO 3 − ) reduction reaction RR) to produce ammonia (NH due their multiple active sites and electron redistribution via strong metal–metal interaction. However, the quantitatively determining atomic configuration of revealing respective roles in NO RR process still challenged. Herein, atomically ordered PdFe L1 2 intermetallic NPs into mesoporous carbon nanofibers (O‐PdFe ‐mCNFs) is reported as an efficient catalyst NH synthesis. Compared face‐centered cubic one, O‐PdFe ‐mCNFs demonstrate a high removal 98.3% within 270 min with large yield rate 1014.2 µmol h −1 cm −2 . The detailed situ theoretical analysis reveals that performance attributed synergetic effect from periodic adjacent Pd‐Fe pair at (110) facet accelerating proton relay, where Fe show preferable stabilization nitrogen−oxygen (*NO) intermediates while Pd serve reservoir *NO hydrogenation. Moreover, d ‐ orbital hybridization tunes ‐band center alloy effectively modulates adsorption energy *NO. This electrocatalyst design offers new avenue developing highly multifunctional catalysts.

Язык: Английский

Процитировано

14