A Nitrogen Battery Electrode involving Eight‐Electron Transfer per Nitrogen for Energy Storage DOI Creative Commons
Haifeng Jiang, Gao‐Feng Chen, Guangtong Hai

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(30)

Опубликована: Май 26, 2023

Abstract Redox flow batteries have been discussed as scalable and simple stationary energy storage devices. However, currently developed systems encounter less competitive density high costs, restricting their wider application. There is a lack of appropriate redox chemistry, preferably based on active materials that are abundant in nature show solubility aqueous electrolytes. A nitrogen‐centered cycle operating between the limiting species ammonia nitrate via an eight‐electron reaction stayed practically unnoticed, albeit its ubiquity biological processes. Ammonia or world‐scale chemicals with solubility, then comparably safe. We demonstrate here successful implementation such nitrogen‐based transfer catholyte for Zn‐based batteries, which continuously worked 12.9 days 930 charging‐discharging cycles. very 577 Wh L −1 can be reached, well above most reported (e.g. 8 times standard Zn‐bromide battery), demonstrating nitrogen offer promising cathodic chemistry safe, affordable, high‐energy‐density

Язык: Английский

Enabled Efficient Ammonia Synthesis and Energy Supply in a Zinc–Nitrate Battery System by Separating Nitrate Reduction Process into Two Stages DOI Creative Commons
Haifeng Jiang, Gao‐Feng Chen, Aleksandr Savateev

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 2, 2023

The aqueous electrocatalytic reduction of NO3- into NH3 (NitrRR) presents a sustainable route applicable to production and potentially energy storage. However, the NitrRR involves directly eight-electron transfer process generally required large overpotential (<-0.2 V versus reversible hydrogen electrode (vs. RHE)) reach optimal efficiency. Here, inspired by biological nitrate respiration, was separated two stages along [2+6]-electron pathway alleviate kinetic barrier. system employed Cu nanowire catalyst produces NO2- with current efficiencies 91.5 % 100 %, respectively at lower overpotentials (>+0.1 vs. RHE). high efficiency for such further explored in zinc-nitrate battery. This battery could be specified output voltage 0.70 V, an average density 566.7 Wh L-1 10 mA cm-2 power 14.1 mW , which is well beyond all previously reported similar concepts.

Язык: Английский

Процитировано

176
Recent progress and strategies on the design of catalysts for electrochemical ammonia synthesis from nitrate reduction DOI
Wei Song,

Luchao Yue,

Xiaoya Fan

и другие.

Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(12), С. 3489 - 3514

Опубликована: Янв. 1, 2023

Ammonia (NH3) is an essential raw material in the production of fertilizers and a promising carbon-free energy carrier, however, its synthesis still depends on energy- capital-intensive Haber–Bosch process. Recently, electrochemical N2 reduction reaction has attracted significant interest as emerging method for NH3 under ambient conditions. However, limited solubility aqueous electrolyte strong NN bonds result low yield rate, inferior faradaic efficiency unsatisfactory selectivity, impeding further practical application. Considering high water nitrate (NO3−), NO3− (NO3−RR) become fascinating route achieving sustainable NH3, enormous progress been made this field. As consequence, review discusses mechanism systematically summarizes recent development electrocatalysts NO3−RR, including noble-metal-based materials, single-atom metal catalysts, transition-metal-based catalysts. Diverse design strategies catalysts to boost NO3−RR performance, such defect engineering, rational structure design, strain engineering constructing heterostructures, are discussed. This followed by illustration how robust understanding optimization affords fundamental insights into efficiency, selectivity electrocatalysts. Finally, we conclude with future perspectives critical issues, challenges research directions high-efficiency selective NH3.

Язык: Английский

Процитировано

125
Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia DOI

Zunjie Zhang,

Yang Liu, Xiaozhi Su

и другие.

Nano Research, Год журнала: 2023, Номер 16(5), С. 6632 - 6641

Опубликована: Март 20, 2023

Язык: Английский

Процитировано

86
Self‐Supported Pd Nanorod Arrays for High‐Efficient Nitrate Electroreduction to Ammonia DOI
Heng Guo, Mengyue Li,

Yuantao Yang

и другие.

Small, Год журнала: 2023, Номер 19(10)

Опубликована: Янв. 22, 2023

Electrochemical nitrate (NO3- ) reduction to ammonia (NH3 offers a promising pathway recover NO3- pollutants from industrial wastewater that can balance the nitrogen cycle and sustainable green NH3 production. However, efficiency of electrocatalytic synthesis remains low for most electrocatalysts due complex reaction processes severe hydrogen precipitation reaction. Herein, high performance RR) is demonstrated on self-supported Pd nanorod arrays in porous nickel framework foam (Pd/NF). It provides lot active sites H* adsorption activation leading remarkable yield rate 1.52 mmol cm-2 h-1 Faradaic 78% at -1.4 V versus RHE. Notably, it maintains over 50 cycles 25 h showing good stability. Remarkably, large-area Pd/NF electrode (25 cm2 shows 174.25 mg , be candidate device application. In situ FTIR spectroscopy density functional theory calculations analysis confirm enrichment effect nanorods encourages H species following hydrogenation mechanism. This work brings useful strategy designing RR catalysts with customizable compositions.

Язык: Английский

Процитировано

77
Rare earth oxide based electrocatalysts: synthesis, properties and applications DOI
Yong Jiang, Hao Fu, Zhong Liang

и другие.

Chemical Society Reviews, Год журнала: 2023, Номер 53(2), С. 714 - 763

Опубликована: Дек. 18, 2023

The synthesis, properties and applications of rare earth oxide based electrocatalysts in electrocatalysis reactions.

Язык: Английский

Процитировано

71
Electrocatalytic nitrate-to-ammonia conversion on CoO/CuO nanoarrays using Zn–nitrate batteries DOI
Shanshan Chen, Gaocan Qi,

Ruilian Yin

и другие.

Nanoscale, Год журнала: 2023, Номер 15(48), С. 19577 - 19585

Опубликована: Янв. 1, 2023

Zn-NO3- batteries can generate electricity while producing NH3 in an environmentally friendly manner, making them a very promising device. However, the conversion of NO3- to involves proton-assisted 8-electron (8e-) transfer process with high kinetic barrier, requiring high-performance catalysts realize potential applications this technology. Herein, we propose heterostructured CoO/CuO nanoarray electrocatalyst prepared on copper foam (CoO/CuO-NA/CF) that electrocatalytically and efficiently convert at low achieves maximum yield 296.9 μmol h-1 cm-2 Faraday efficiency (FE) 92.9% -0.2 V vs. reversible hydrogen electrode (RHE). Impressively, battery based monolithic CoO/CuO-NA/CF delivers 60.3 cm-2, FENH3 82.0%, power density 4.3 mW cm-2. This study provides paradigm for catalyst preparation energy-efficient production simultaneously generating electrical energy.

Язык: Английский

Процитировано

64
Oxygen Vacancies‐Rich Metal Oxide for Electrocatalytic Nitrogen Cycle DOI
Xiaoxiao Wei, Chen Chen, Xian‐Zhu Fu

и другие.

Advanced Energy Materials, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 13, 2023

Abstract The development of industry and agriculture has been accompanied by an artificially imbalanced nitrogen cycle, which threatens human health ecological environments. Electrocatalytic systems have emerged as a sustainable way converting nitrogen‐containing molecules into high value‐added chemicals. However, the construction high‐performance electrocatalysts remains challenging. oxygen vacancy engineering strategy promoted more research efforts to explore structure‐activity relationship between catalytic activity vacancies. This review systematically summarizes recent vacancies‐rich metal oxides for electro‐catalyzing cycling systems, involving electrocatalytic nitrate reduction reaction, nitric oxide C─N coupling, urea oxidation reaction. First, methods characterization vacancies are summarized. Then, effect on is discussed in terms regulating electronic structures electrocatalysts, improving electroconductivity catalysts, lowing energy barrier, strengthening adsorption activation intermediate species. Finally, future directions cycle anticipated.

Язык: Английский

Процитировано

62
Electrocatalytic Nitrate Reduction on Metallic CoNi‐Terminated Catalyst with Industrial‐Level Current Density in Neutral Medium DOI
Yingying Wei, Jingjing Huang, Hong Chen

и другие.

Advanced Materials, Год журнала: 2024, Номер 36(30)

Опубликована: Май 9, 2024

Abstract Green ammonia synthesis through electrocatalytic nitrate reduction reaction (eNO 3 RR) can serve as an effective alternative to the traditional energy‐intensive Haber‐Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges eNO RR. Herein, with guidance of theoretical calculation, a metallic CoNi‐terminated catalyst is successfully designed and constructed on copper foam, which achieves FE up 100% under industrial‐level very low overpotential (−0.15 V versus reversible hydrogen electrode) medium. Multiple characterization results have confirmed that maintained metal atom‐terminated surface interaction atoms plays crucial role reducing density. By constructing homemade gas stripping absorption device, complete conversion process for high‐purity ammonium products demonstrated, displaying potential practical application. This work suggests sustainable promising toward directly converting nitrate‐containing pollutant solutions into nitrogen fertilizers.

Язык: Английский

Процитировано

43
Surface Oxygen Vacancies Induced by Calcium Substitution in Macroporous La2Ce2–xCaxO7−δ Catalysts for Boosting Low-Temperature Oxidative Coupling of Methane DOI
Tongtong Wu, Peng Zhang, Yuechang Wei

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(3), С. 1882 - 1902

Опубликована: Янв. 20, 2024

Surface oxygen vacancies in the catalysts play a key role improving catalytic performances for low-temperature oxidative coupling of methane (OCM). Herein, macroporous La2Ce2–xCaxO7−δ (A2B2O7-type) with disordered defective cubic fluorite phased structure were prepared by citric acid sol–gel method. The improved accessibility reactants (O2 and CH4) to active sites. partial substitution B site (Ce) low-valence calcium (Ca) ions induced formation surface vacancies, which facilitated adsorption activation O2 molecules generate species (O2– species). O2– can boost CH4 govern following step dehydrogenation C2H6 C2H4. have high activity OCM, La2Ce1.3Ca0.7O7−δ catalyst highest density exhibits during OCM into C2H4 (C2) products, i.e., its conversion, selectivity, yield C2 products at 600 °C are 31.0, 65.6, 20.3%, respectively. Based on results multiple experimental characterizations functional theory calculations, mechanism reaction is proposed: Ce Ca significantly promote critical steps C–H bond breaking C–C reaction. It important design high-efficiency practical applications.

Язык: Английский

Процитировано

21
Two‐dimensional Cu Plates with Steady Fluid Fields for High‐rate Nitrate Electroreduction to Ammonia and Efficient Zn‐Nitrate Batteries DOI

Limin Zhou,

Xueqiu Chen,

Shaojun Zhu

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(18)

Опубликована: Фев. 17, 2024

Abstract Nitrate electroreduction reaction (eNO 3 − RR) to ammonia (NH ) provides a promising strategy for nitrogen utilization, while achieving high selectivity and durability at an industrial scale has remained challenging. Herein, we demonstrated that the performance of eNO RR could be significantly boosted by introducing two‐dimensional Cu plates as electrocatalysts eliminating general carrier gas construct steady fluid field. The developed setup provided superior NH Faradaic efficiency (FE) 99 %, exceptional long‐term electrolysis 120 h 200 mA cm −2 , record‐high yield rate 3.14 mmol −1 . Furthermore, proposed was successfully extended Zn‐nitrate battery system, providing power density 12.09 mW FE 85.4 outperforming state‐of‐the‐art catalysts. Coupled with COMSOL multiphysics simulations in situ infrared spectroscopy, main contributor high‐efficiency production field timely rejuvenate electrocatalyst surface during electrocatalysis.

Язык: Английский

Процитировано

19