Regulating the d-Band Center of Metal–Organic Frameworks for Efficient Nitrate Reduction Reaction and Zinc-Nitrate Battery DOI

Yuanhui Yao,

Xiaofei Wei,

Haiqiao Zhou

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(21), С. 16205 - 16213

Опубликована: Окт. 18, 2024

The electrochemical reduction of nitrate ions to valuable ammonia enables the recovery pollutants from industrial wastewater, thereby synchronously balancing nitrogen cycle and achieving NH3 production. However, currently reported electrocatalysts still suffer low yield rate, Faradaic inefficiency, partial current density. Herein, a strategy based on regulation d-band center by Ru doping is presented boost Theoretical calculations unravel that dopant in Ni metal–organic framework shifts neighboring sites upward, optimizing adsorption strength N-intermediates, resulting greatly enhanced reaction performance. synthesized Ru-doped rod array electrode delivers rate 1.31 mmol h–1 cm–2 efficiency 91.5% at −0.6 V versus reversible hydrogen electrode, as well good cycling stability. In view multielectron transfer electrocatalytic activity, Zn-NO3– battery assembled this Zn anode, which high open-circuit voltage 1.421 maximum output power density 4.99 mW cm–2, demonstrating potential application value.

Язык: Английский

Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis DOI Creative Commons
Jie Liang, Qian Liu, Abdulmohsen Ali Alshehri

и другие.

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120010 - e9120010

Опубликована: Май 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Язык: Английский

Процитировано

351

Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction DOI Creative Commons
Jie Liang, Zixiao Li, Longcheng Zhang

и другие.

Chem, Год журнала: 2023, Номер 9(7), С. 1768 - 1827

Опубликована: Июнь 21, 2023

Язык: Английский

Процитировано

281

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond DOI
Yuecheng Xiong, Yunhao Wang, Jingwen Zhou

и другие.

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

Процитировано

237

Interfacial polarization in metal-organic framework reconstructed Cu/Pd/CuOx multi-phase heterostructures for electrocatalytic nitrate reduction to ammonia DOI

Tianlun Ren,

Zuan Yu,

Hongjie Yu

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 318, С. 121805 - 121805

Опубликована: Июль 28, 2022

Язык: Английский

Процитировано

157

Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia DOI
Di Liu, Lulu Qiao,

Shuyang Peng

и другие.

Advanced Functional Materials, Год журнала: 2023, Номер 33(43)

Опубликована: Июнь 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Язык: Английский

Процитировано

153

High-Efficiency Electrochemical Nitrate Reduction to Ammonia on a Co3O4 Nanoarray Catalyst with Cobalt Vacancies DOI
Zhiqin Deng, Chaoqun Ma, Zerong Li

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2022, Номер 14(41), С. 46595 - 46602

Опубликована: Окт. 5, 2022

Electrocatalytic nitrate reduction reaction (NO3RR) affords a bifunctional character in the carbon-free ammonia synthesis and remission of pollution water. Here, we fabricated Co3O4 nanosheet array with cobalt vacancies on carbon cloth (vCo-Co3O4/CC) by situ etching aluminum-doped Co3O4/CC, which exhibits an excellent Faradaic efficiency 97.2% large NH3 yield as high 517.5 μmol h-1 cm-2, better than pristine Co3O4/CC. Theoretical calculative results imply that can tune local electronic environment around Co sites Co3O4, increasing charge reducing electron cloud density sites, is thus conducive to adsorption NO3- for greatly enhanced reduction. Furthermore, vCo-Co3O4 (311) facet presents NO3RR activity low energy barrier about 0.63 eV potential-determining step, much smaller (1.3 eV).

Язык: Английский

Процитировано

130

Weakened d–p orbital hybridization inin situreconstructed Ru/β-Co(OH)2heterointerfaces for accelerated ammonia electrosynthesis from nitrates DOI

Weijie Zhu,

Fen Yao,

Qiongfei Wu

и другие.

Energy & Environmental Science, Год журнала: 2023, Номер 16(6), С. 2483 - 2493

Опубликована: Янв. 1, 2023

Electron-deficient Ru sites at Ru/Co(OH) 2 heterointerfaces weaken the d–p orbital hybridization ability and further facilitate desorption of ammonia intermediates, thereby achieving ultrahigh nitrate electroreduction activity towards ammonia.

Язык: Английский

Процитировано

112

Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate DOI

Weidong Wen,

Ping Yan,

Wanping Sun

и другие.

Advanced Functional Materials, Год журнала: 2022, Номер 33(6)

Опубликована: Ноя. 28, 2022

Abstract Electrocatalytic nitrate (NO 3 − ) reduction reaction (NITRR) is an inspiring route for ammonia (NH synthesis at ambient condition. The metallic Cu‐based material with low cost and high activity one of the most promising electrocatalysts NITRR. However, due to weaker atomic H * ‐providing capacity, produced intermediate—nitrite tends accumulate on its surface, leading unsatisfactory NH selectivity Faradic efficiency (FE). Herein, a novel facile O 2 /Ar plasma oxidation subsequent electro‐reduction strategy developed synthesize kind metastable phase Cu. Excitingly, Cu demonstrates superior NITRR performance conventional 4 + (97.8%) FE (99.8%). Density function theory (DFT) calculations reveal that upshift d ‐band center near Fermi level in contributes enhanced activity, while relatively strong adsorption facilitates conversion from NO /NO NOOH /NOH thus ensures FE. Furthermore, when evaluated as cathode Zn‐NO battery, power density (7.56 mW cm −2 yield (76 µmol h −1 are achieved by battery.

Язык: Английский

Процитировано

107

Oxygen vacancies in Co3O4nanoarrays promote nitrate electroreduction for ammonia synthesis DOI
Xiang Xu,

Long Hu,

Zerong Li

и другие.

Sustainable Energy & Fuels, Год журнала: 2022, Номер 6(18), С. 4130 - 4136

Опубликована: Янв. 1, 2022

Oxygen vacancy-enriched Co 3 O 4 nanosheet arrays enable ambient electrosynthesis of NH via nitrate reduction, achieving a faradaic efficiency 96.9% and yield 12 157 μg h −1 cm −2 in 0.1 M NaOH with NO − .

Язык: Английский

Процитировано

106

Energy-efficient electrochemical ammonia production from dilute nitrate solution DOI Creative Commons
Keon‐Han Kim,

Heebin Lee,

Xiaopeng Huang

и другие.

Energy & Environmental Science, Год журнала: 2023, Номер 16(2), С. 663 - 672

Опубликована: Янв. 1, 2023

Highly efficient electrochemical nitrate reduction could be key for sustainable ammonia production. Our NiFe LDH/Cu foam electrode exhibits an NH 3 selectivity of 95.8% with 98.5% conversion.

Язык: Английский

Процитировано

104