The ocean thermal energy conversion (OTEC) system is a promising solution to provide stable electricity supply. Although the available temperature difference in OTEC systems is small, an ammonia/water mixture as worki...The ocean thermal energy conversion (OTEC) system is a promising solution to provide stable electricity supply. Although the available temperature difference in OTEC systems is small, an ammonia/water mixture as working fluid is expected to decrease irreversible losses in the heat exchangers and to improve system performance. However, in actual heat exchangers, an adequate temperature crossing does not occur in the condenser but in the evaporator. Therefore, clarification of this characteristic is important. To date, the logarithmic temperature difference (LMTD) method is used in performance evaluations of OTEC heat exchangers. This method is of limited use if physical properties of fluids vary. A generalized mean temperature difference (GMTD) method is introduced to perform this evaluation. As changes in fluid property values can be considered in the GMTD method, method dependencies on heat exchanger characteristics, effectiveness, and system characteristics can be studied. In particular, GMTD and LMTD using a pure substance were found to be almost equal. Mean temperature differences using mixtures as working fluid were higher in the evaporator, but lower in the condenser, from the GMTD method than from the LMTD method. For higher ammonia concentrations in ammonia/water mixtures, the mean temperature differences from both methods are different.展开更多
Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nont...Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.展开更多
To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and ...To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and acoustic emission(AE)system are used to monitor the rockburst process.The effect of water on sandstone rockburst and the prevention mechanism of water on sandstone rockburst are analyzed from the perspective of energy and failure mode.The results show that the higher the ab-sorption degree,the lower the intensity of the rockburst after absorbing water on single side of sand-stone.This is reflected in the fact that with the increase in the water absorption level,the ejection velocity of rockburst fragments is smaller,the depth of the rockburst pit is shallower,and the AE energy is smaller.Under the water absorption level of 100%,the magnitude of rockburst intensity changes from medium to slight.The prevention mechanism of water on sandstone rockburst is that water reduces the capacity of sandstone to store strain energy and accelerates the expansion of shear cracks,which is not conducive to the occurrence of plate cracking before rockburst,and destroys the conditions for rockburst incubation.展开更多
The development of modern agriculture requires the reduction of water and chemical N fertilizer inputs.Increasing the planting density can maintain higher yields,but also consumes more of these restrictive resources.H...The development of modern agriculture requires the reduction of water and chemical N fertilizer inputs.Increasing the planting density can maintain higher yields,but also consumes more of these restrictive resources.However,whether an increased maize density can compensate for the negative effects of reduced water and N supply on grain yield and N uptake in the arid irrigated areas remains unknown.This study is part of a long-term positioning trial that started in 2016.A split-split plot field experiment of maize was implemented in the arid irrigated area of northwestern China in 2020 to 2021.The treatments included two irrigation levels:local conventional irrigation reduced by 20%(W1,3,240 m^(3)ha^(-1))and local conventional irrigation(W2,4,050 m^(3)ha^(-1));two N application rates:local conventional N reduced by 25%(N1,270 kg ha^(-1))and local conventional N(360 kg ha^(-1));and three planting densities:local conventional density(D1,75,000 plants ha^(-1)),density increased by 30%(D2,97,500 plants ha-1),and density increased by 60%(D3,120,000 plants ha^(-1)).Our results showed that the grain yield and aboveground N accumulation of maize were lower under the reduced water and N inputs,but increasing the maize density by 30% can compensate for the reductions of grain yield and aboveground N accumulation caused by the reduced water and N supply.When water was reduced while the N application rate remained unchanged,increasing the planting density by 30% enhanced grain yield by 13.9% and aboveground N accumulation by 15.3%.Under reduced water and N inputs,increasing the maize density by 30% enhanced N uptake efficiency and N partial factor productivity,and it also compensated for the N harvest index and N metabolic related enzyme activities.Compared with W2N2D1,the N uptake efficiency and N partial factor productivity increased by 28.6 and 17.6%under W1N1D2.W1N2D2 had 8.4% higher N uptake efficiency and 13.9% higher N partial factor productivity than W2N2D1.W1N2D2 improved urease activity and nitrate reductase activity by 5.4% at the R2(blister)stage and 19.6% at the V6(6th leaf)stage,and increased net income and the benefit:cost ratio by 22.1 and 16.7%,respectively.W1N1D2 and W1N2D2 reduced the nitrate nitrogen and ammoniacal nitrogen contents at the R6 stage in the 40-100 cm soil layer,compared with W2N2D1.In summary,increasing the planting density by 30% can compensate for the loss of grain yield and aboveground N accumulation under reduced water and N inputs.Meanwhile,increasing the maize density by 30% improved grain yield and aboveground N accumulation when water was reduced by 20% while the N application rate remained constant in arid irrigation areas.展开更多
A submerged cavitation water jet(SCWJ)is an effective method to recycle solid propellant from obsolete solid engines by the breaking method.Solid propellant's breaking modes and mechanical process under SCWJ impac...A submerged cavitation water jet(SCWJ)is an effective method to recycle solid propellant from obsolete solid engines by the breaking method.Solid propellant's breaking modes and mechanical process under SCWJ impact are unclear.This study aims to understand those impact breaking mechanisms.The hydroxyl-terminated polybutadiene(HTPB)propellant was chosen as the research material,and a self-designed test system was used to conduct impact tests at four different working pressures.The high-speed camera characterized crack propagation,and the DIC method calculated strain change during the impact process.Besides,micro and macro fracture morphologies were characterized by scanning electron microscope(SEM)and computed tomography(CT)scanning.The results reveal that the compressive strain concentration region locates right below the nozzle,and the shear strain region distributes symmetrically with the jet axis,which increases to 4% at first 16th ms,the compressive strain rises to 2% and 6% in the axial and transverse direction,respectively.The two tensile cracks formed first at the compression strain concentrate region,and there generate many shear cracks around the tensile cracks,and those shear cracks that develop and aggregate cause the cracks to become wider and cut through the tensile cracks,forming the tensile-shear cracks and the impact parts eventually fail.The HTPB propellant forms a breaking hole shaped conical after impact 10 s.The mass loss increases by 17 times at maximum,with the working pressure increasing by three times.Meanwhile,the damage value of the breaking hole remaining on the surface increases by 7.8 times while 2.9 times in the depth of the breaking hole.The breaking efficiency is closely affected by working pressures.The failure modes of HTPB impacted by SCWJ are classified as tensile crack-dominated and tensile-shear crack-dominated damage mechanisms.展开更多
Green hydrogen(H_(2))produced by renewable energy powered alkaline water electrolysis is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.However,efficient and economic...Green hydrogen(H_(2))produced by renewable energy powered alkaline water electrolysis is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.However,efficient and economic H_(2) production by alkaline water electrolysis is hindered by the sluggish hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Therefore,it is imperative to design and fabricate high-active and low-cost non-precious metal catalysts to improve the HER and OER performance,which affects the energy efficiency of alkaline water electrolysis.Ni_(3)S_(2) with the heazlewoodite structure is a potential electrocatalyst with near-metal conductivity due to the Ni–Ni metal network.Here,the review comprehensively presents the recent progress of Ni_(3)S_(2)-based electrocatalysts for alkaline water electrocatalysis.Herein,the HER and OER mechanisms,performance evaluation criteria,preparation methods,and strategies for performance improvement of Ni_(3)S_(2)-based electrocatalysts are discussed.The challenges and perspectives are also analyzed.展开更多
In this article, the names of 3 varieties of Monarda didyma L., which are considered to be introduced species, some indicators of the water regime in the climatic conditions of Uzbekistan: the amount of water in the l...In this article, the names of 3 varieties of Monarda didyma L., which are considered to be introduced species, some indicators of the water regime in the climatic conditions of Uzbekistan: the amount of water in the leaves, water deficit, water storage capacity were studied in spring and summer, and seasonal changes were determined. According to these indicators of the water regime, the studied varieties belong to the labile water regime, high green mass (centner), seed yield (how many grams), resistance to diseases and pests have been determined, which shows that it is promising for introduction in the conditions of our republic. Therefore, it is recommended to breed these varieties in the foothills and hilly regions of Uzbekistan, where the amount of precipitation is more than 400 - 500 mm.展开更多
A multi-faceted Case Area Targeted Intervention (CATI) approach emphasizing the integration of Water, Sanitation and Hygiene (WASH) interventions and Oral Cholera Vaccine (OCV) campaign was employed to respond to the ...A multi-faceted Case Area Targeted Intervention (CATI) approach emphasizing the integration of Water, Sanitation and Hygiene (WASH) interventions and Oral Cholera Vaccine (OCV) campaign was employed to respond to the outbreak of cholera in Garissa County. Drinking water sources in areas heavily impacted by cholera were systematically mapped and tested for microbiological quality. The quality assessment was carried out in April 2023 during an ongoing cholera outbreak in the county. A total of 109 samples were collected and tested for thermotolerant coliforms and other in situ parameters. The finding revealed that more than 87% of the samples did not meet the World Health Organization (WHO) standard for thermotolerant coliforms;and 30% had turbidity values above the recommended threshold values. None of the 109 samples had any traceable residual chlorine. Following these findings, the county government implemented the targeted interventions which resulted in a positive impact in the fight against cholera. The WHO supported key interventions which included capacity building in water quality monitoring and prepositioning of critical WASH commodities to the cholera affected areas.展开更多
The primary objective of this study was to design and size a sustainable sanitation solution for the Ndiebene Gandiol 1 school located in the eponymous commune in northern Senegal. Field investigations led to the coll...The primary objective of this study was to design and size a sustainable sanitation solution for the Ndiebene Gandiol 1 school located in the eponymous commune in northern Senegal. Field investigations led to the collection of wastewater samples. Their analysis revealed specific pollutant loads, including loads of BOD5 3.6966 kgO<sub>2</sub>/day and COD of 12.8775 kgO<sub>2</sub>/day, which were central to the design phase. Following a rigorous assessment of the existing sanitation infrastructure, constructed wetland (CWs) emerged as the most appropriate ecological solution. This system, valued for its ability to effectively remove contaminants, was tailored to the specific needs of the site. Consequently, the final design of the filter extends over 217.16 m<sup>2</sup>, divided into two cells of 108.58 m<sup>2</sup> each, with dimensions of 12.77 m in length and 8.5 m in width. The depth of the filtering medium is approximately 0.60 m, meeting the standards while ensuring maximized purification. Typha, an indigenous and prolific plant known for its purification abilities, was selected as the filtering agent. Concurrently, non-crushed gravel was chosen for its proven filtration capacity. This study is the result of a combination of scientific rigor and design expertise. It provides a holistic view of sanitation for Ndiebene Gandiol. The technical specifications and dimensions of the constructed wetland filter embody an approach that marries indepth analysis and practical application, all aimed at delivering an effective and long-lasting solution to the local sanitation challenges. By integrating precise scientific data with sanitation design expertise, this study delivers a holistic solution for Ndiebene Gandiol. The detailed dimensions and specifications of the constructed wetland filter reflect a methodology that combines meticulous analysis with practical adaptation, aiming to provide an effective and sustainable response to the challenges of rural and school sanitation in the northern region of Senegal.展开更多
For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based ...For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based species(N—C)/NOx is optimized using the Non-dominated Sorting Genetic Algorithm II(NSGA-II)with 200 generations.The optimized mechanism(named as 937b)is validated against combustion characteristics of ammonia/methane(which is used to examine the accuracy of N—C interactions)and ammonia/diesel blends.The ignition delay times(IDTs),the laminar flame speeds and most of key intermediate species during the combustion of ammonia/methane blends can be accurately simulated by 937b under a wide range of conditions.As for ammonia/diesel blends with various diesel energy fractions,reasonable predictions on the IDTs under pressures from 1.0 MPa to5.0 MPa as well as the laminar flame speeds are also achieved by 937b.In particular,with regard to the IDT simulations of ammonia/diesel blends,937b makes progress in both aspects of overall accuracy and computational efficiency,compared to a detailed ammonia/diesel mechanism.Further kinetic analysis reveals that the reaction pathway of ammonia during the combustion of ammonia/diesel blend mainly differs in the tendencies of oxygen additions to NH_2 and NH with different equivalence ratios.展开更多
For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions...For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.展开更多
The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for ...The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.展开更多
The knowledge of the residence time of formation water is fundamental to understanding the subsurface flow and hydrological setting.To better identify the origin and evolution of coal seam water and its impact on gas ...The knowledge of the residence time of formation water is fundamental to understanding the subsurface flow and hydrological setting.To better identify the origin and evolution of coal seam water and its impact on gas storage and production,this study collected coalbed methane co-produced water in the southeast Qinshui Basin and detected chemical and isotopic compositions,especially 36Cl and 129I concentrations.The calculated tracer ages of 129I(5.2–50.6 Ma)and 36Cl(0.13–0.76 Ma)are significantly younger than the age of coal-bearing formation(Pennsylvanian-Cisuralian),indicating freshwater recharge after coal deposition.The model that utilises 129I/I and 36Cl/Cl ratios to constrain the timing of recharge and the proportion of recharge water reveals that over 60%of pre-anthropogenic meteoric water entered coal seams since 10 Ma and mixed with residue initial deposition water,corresponding to the basin inversion in Cenozoic.The spatial distribution of major ion concentrations reveals the primary recharge pathway for meteoric water from coal outcrops at the eastern margin to the basin center.This study demonstrates the occurrence of higher gas production rates from wells that accept water recharge in recent times and suggests the possible potential of the non-stagnant zones for high gas production.展开更多
Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the...Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon emissions.Renewables-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen production.Conventional water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen species.By virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas safely.Decoupled electrolysis has accelerated the development ofwater electrolysis technology for H_(2) production.However,itis still lack of a comprehensive and in-depth review in this field based on different types of RMs.This review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past decade.Several representative examples are then dis-played in detail according to the differences in the RMs.The rational choice and design of RMs have also been emphasized.Subsequently,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial photosynthesis.Finally,thekey characteristics and disadvantages of each type of mediator are sum-marized in depth.In addition,we present an outlook for future directions in decoupled water splitting.Thus,the flexibility in the design of mediators provides huge space for improving this electrochemical technology.@2024 Science Press and Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by ELSEVIER B.V.and Science Press.All rights reserved.展开更多
As a typical region with high water demand for agricultural production,understanding the spatiotemporal surface water changes in Northeast China is critical for water resources management and sustainable development.H...As a typical region with high water demand for agricultural production,understanding the spatiotemporal surface water changes in Northeast China is critical for water resources management and sustainable development.However,the long-term variation characteristics of surface water of different water body types in Northeast China remain rarely explored.This study investigated how surface water bodies of different types(e.g.,lake,reservoir,river,coastal aquaculture,marsh wetland,ephemeral water) changed during1999–2020 in Northeast China based on various remote sensing-based datasets.The results showed that surface water in Northeast China grew dramatically in the past two decades,with an equivalent area increasing from 24 394 km^(2) in 1999 to 34 595 km^(2) in 2020.The surge of ephemeral water is the primary driver of surface water expansion,which could ascribe to shifted precipitation pattern.Marsh wetlands,rivers,and reservoirs experienced a similar trend,with an approximate 20% increase at the interdecadal scale.By contrast,coastal aquacultures and natural lakes remain relatively stable.This study is expected to provide a more comprehensive investigation of the surface water variability in Northeast China and has important practical significance for the scientific management of different types of surface water.展开更多
Virtual water trade(VWT)provides a new perspective for alleviating water crisis and has thus attracted widespread attention.However,the heterogeneity of virtual water trade inside and outside the river basin and its i...Virtual water trade(VWT)provides a new perspective for alleviating water crisis and has thus attracted widespread attention.However,the heterogeneity of virtual water trade inside and outside the river basin and its influencing factors remains further study.In this study,for better investigating the pattern and heterogeneity of virtual water trade inside and outside provincial regions along the Yellow River Basin in 2015 using the input-output model(MRIO),we proposed two new concepts,i.e.,virtual water surplus and virtual water deficit,and then used the Logarithmic Mean Divisia Index(LMDI)model to identify the inherent mechanism of the imbalance of virtual water trade between provincial regions along the Yellow River Basin and the other four regions in China.The results show that:1)in provincial regions along the Yellow River Basin,the less developed the economy was,the larger the contribution of the agricultural sector in virtual water trade,while the smaller the contribution of the industrial sector.2)Due to the large output of agricultural products,the upstream and midstream provincial regions of the Yellow River Basin had a virtual water surplus,with a net outflow of virtual water of 2.7×10^(8) m^(3) and 0.9×10^(8) m^(3),respectively.3)provincial regions along the Yellow River Basin were in a virtual water deficit with the rest of China,and the decisive factor was the active degree of trade with the outside.This study would be beneficial to illuminate the trade-related water use issues in provincial regions along the Yellow River Basin,which has farreaching practical signific-ance for alleviating water scarcity.展开更多
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the...Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.展开更多
The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia syn...The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.展开更多
Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and i...Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and is regarded as a future technology for production of CO_(2)-free pure hydrogen.Herein,a heterostructural Pt-Ir dual-layer electrode is developed and shown to achieve successful long-term operation in an ammonia electrolyzer with an anion exchange membrane(AEM).This electrolyzer consisted of eight membra ne electrode assemblies(MEAs)with a total geometric area of 200 cm~2 on the anode side,which resulted in a hydrogen production rate of 25 L h~(-1).We observed the degradation in MEA performance attributed to changes in the anode catalyst layer during hydrogen production via ammonia electrolysis.Furthermore,we demonstrated the relationship between the ammonia oxidation reaction(AOR)and the oxygen evolution reaction(OER).展开更多
文摘The ocean thermal energy conversion (OTEC) system is a promising solution to provide stable electricity supply. Although the available temperature difference in OTEC systems is small, an ammonia/water mixture as working fluid is expected to decrease irreversible losses in the heat exchangers and to improve system performance. However, in actual heat exchangers, an adequate temperature crossing does not occur in the condenser but in the evaporator. Therefore, clarification of this characteristic is important. To date, the logarithmic temperature difference (LMTD) method is used in performance evaluations of OTEC heat exchangers. This method is of limited use if physical properties of fluids vary. A generalized mean temperature difference (GMTD) method is introduced to perform this evaluation. As changes in fluid property values can be considered in the GMTD method, method dependencies on heat exchanger characteristics, effectiveness, and system characteristics can be studied. In particular, GMTD and LMTD using a pure substance were found to be almost equal. Mean temperature differences using mixtures as working fluid were higher in the evaporator, but lower in the condenser, from the GMTD method than from the LMTD method. For higher ammonia concentrations in ammonia/water mixtures, the mean temperature differences from both methods are different.
基金partially supported by the Australian Research Council(ARC)the National Science Fund for Distinguished Young Scholars(grant number 51925703)。
文摘Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.
基金The financial support from the National Natural Science Foun-dation of China(Grant Nos.52074299 and 41941018)the Fundamental Research Funds for the Central Universities of China(Grant No.2023JCCXSB02)are gratefully acknowledged.
文摘To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and acoustic emission(AE)system are used to monitor the rockburst process.The effect of water on sandstone rockburst and the prevention mechanism of water on sandstone rockburst are analyzed from the perspective of energy and failure mode.The results show that the higher the ab-sorption degree,the lower the intensity of the rockburst after absorbing water on single side of sand-stone.This is reflected in the fact that with the increase in the water absorption level,the ejection velocity of rockburst fragments is smaller,the depth of the rockburst pit is shallower,and the AE energy is smaller.Under the water absorption level of 100%,the magnitude of rockburst intensity changes from medium to slight.The prevention mechanism of water on sandstone rockburst is that water reduces the capacity of sandstone to store strain energy and accelerates the expansion of shear cracks,which is not conducive to the occurrence of plate cracking before rockburst,and destroys the conditions for rockburst incubation.
基金financial support of the National Natural Science Foundation of China(U21A20218 and 32101857)the‘Double First-Class’Key Scientific Research Project of Education Department in Gansu Province,China(GSSYLXM-02)+1 种基金the Fuxi Young Talents Fund of Gansu Agricultural University,China(Gaufx03Y10)the“Innovation Star”Program of Graduate Students in 2023 of Gansu Province,China(2023CXZX681)。
文摘The development of modern agriculture requires the reduction of water and chemical N fertilizer inputs.Increasing the planting density can maintain higher yields,but also consumes more of these restrictive resources.However,whether an increased maize density can compensate for the negative effects of reduced water and N supply on grain yield and N uptake in the arid irrigated areas remains unknown.This study is part of a long-term positioning trial that started in 2016.A split-split plot field experiment of maize was implemented in the arid irrigated area of northwestern China in 2020 to 2021.The treatments included two irrigation levels:local conventional irrigation reduced by 20%(W1,3,240 m^(3)ha^(-1))and local conventional irrigation(W2,4,050 m^(3)ha^(-1));two N application rates:local conventional N reduced by 25%(N1,270 kg ha^(-1))and local conventional N(360 kg ha^(-1));and three planting densities:local conventional density(D1,75,000 plants ha^(-1)),density increased by 30%(D2,97,500 plants ha-1),and density increased by 60%(D3,120,000 plants ha^(-1)).Our results showed that the grain yield and aboveground N accumulation of maize were lower under the reduced water and N inputs,but increasing the maize density by 30% can compensate for the reductions of grain yield and aboveground N accumulation caused by the reduced water and N supply.When water was reduced while the N application rate remained unchanged,increasing the planting density by 30% enhanced grain yield by 13.9% and aboveground N accumulation by 15.3%.Under reduced water and N inputs,increasing the maize density by 30% enhanced N uptake efficiency and N partial factor productivity,and it also compensated for the N harvest index and N metabolic related enzyme activities.Compared with W2N2D1,the N uptake efficiency and N partial factor productivity increased by 28.6 and 17.6%under W1N1D2.W1N2D2 had 8.4% higher N uptake efficiency and 13.9% higher N partial factor productivity than W2N2D1.W1N2D2 improved urease activity and nitrate reductase activity by 5.4% at the R2(blister)stage and 19.6% at the V6(6th leaf)stage,and increased net income and the benefit:cost ratio by 22.1 and 16.7%,respectively.W1N1D2 and W1N2D2 reduced the nitrate nitrogen and ammoniacal nitrogen contents at the R6 stage in the 40-100 cm soil layer,compared with W2N2D1.In summary,increasing the planting density by 30% can compensate for the loss of grain yield and aboveground N accumulation under reduced water and N inputs.Meanwhile,increasing the maize density by 30% improved grain yield and aboveground N accumulation when water was reduced by 20% while the N application rate remained constant in arid irrigation areas.
基金supported by the Program for National Defense Science and Technology Foundation Strengtheningthe Youth Foundation of Rocket Force University of Engineering(Grant No.2021QN-B014)。
文摘A submerged cavitation water jet(SCWJ)is an effective method to recycle solid propellant from obsolete solid engines by the breaking method.Solid propellant's breaking modes and mechanical process under SCWJ impact are unclear.This study aims to understand those impact breaking mechanisms.The hydroxyl-terminated polybutadiene(HTPB)propellant was chosen as the research material,and a self-designed test system was used to conduct impact tests at four different working pressures.The high-speed camera characterized crack propagation,and the DIC method calculated strain change during the impact process.Besides,micro and macro fracture morphologies were characterized by scanning electron microscope(SEM)and computed tomography(CT)scanning.The results reveal that the compressive strain concentration region locates right below the nozzle,and the shear strain region distributes symmetrically with the jet axis,which increases to 4% at first 16th ms,the compressive strain rises to 2% and 6% in the axial and transverse direction,respectively.The two tensile cracks formed first at the compression strain concentrate region,and there generate many shear cracks around the tensile cracks,and those shear cracks that develop and aggregate cause the cracks to become wider and cut through the tensile cracks,forming the tensile-shear cracks and the impact parts eventually fail.The HTPB propellant forms a breaking hole shaped conical after impact 10 s.The mass loss increases by 17 times at maximum,with the working pressure increasing by three times.Meanwhile,the damage value of the breaking hole remaining on the surface increases by 7.8 times while 2.9 times in the depth of the breaking hole.The breaking efficiency is closely affected by working pressures.The failure modes of HTPB impacted by SCWJ are classified as tensile crack-dominated and tensile-shear crack-dominated damage mechanisms.
基金supported by the National Key Research and Development Program(No.2022YFB4202200)the Fundamental Research Funds for the Central Universities.
文摘Green hydrogen(H_(2))produced by renewable energy powered alkaline water electrolysis is a promising alternative to fossil fuels due to its high energy density with zero-carbon emissions.However,efficient and economic H_(2) production by alkaline water electrolysis is hindered by the sluggish hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Therefore,it is imperative to design and fabricate high-active and low-cost non-precious metal catalysts to improve the HER and OER performance,which affects the energy efficiency of alkaline water electrolysis.Ni_(3)S_(2) with the heazlewoodite structure is a potential electrocatalyst with near-metal conductivity due to the Ni–Ni metal network.Here,the review comprehensively presents the recent progress of Ni_(3)S_(2)-based electrocatalysts for alkaline water electrocatalysis.Herein,the HER and OER mechanisms,performance evaluation criteria,preparation methods,and strategies for performance improvement of Ni_(3)S_(2)-based electrocatalysts are discussed.The challenges and perspectives are also analyzed.
文摘In this article, the names of 3 varieties of Monarda didyma L., which are considered to be introduced species, some indicators of the water regime in the climatic conditions of Uzbekistan: the amount of water in the leaves, water deficit, water storage capacity were studied in spring and summer, and seasonal changes were determined. According to these indicators of the water regime, the studied varieties belong to the labile water regime, high green mass (centner), seed yield (how many grams), resistance to diseases and pests have been determined, which shows that it is promising for introduction in the conditions of our republic. Therefore, it is recommended to breed these varieties in the foothills and hilly regions of Uzbekistan, where the amount of precipitation is more than 400 - 500 mm.
文摘A multi-faceted Case Area Targeted Intervention (CATI) approach emphasizing the integration of Water, Sanitation and Hygiene (WASH) interventions and Oral Cholera Vaccine (OCV) campaign was employed to respond to the outbreak of cholera in Garissa County. Drinking water sources in areas heavily impacted by cholera were systematically mapped and tested for microbiological quality. The quality assessment was carried out in April 2023 during an ongoing cholera outbreak in the county. A total of 109 samples were collected and tested for thermotolerant coliforms and other in situ parameters. The finding revealed that more than 87% of the samples did not meet the World Health Organization (WHO) standard for thermotolerant coliforms;and 30% had turbidity values above the recommended threshold values. None of the 109 samples had any traceable residual chlorine. Following these findings, the county government implemented the targeted interventions which resulted in a positive impact in the fight against cholera. The WHO supported key interventions which included capacity building in water quality monitoring and prepositioning of critical WASH commodities to the cholera affected areas.
文摘The primary objective of this study was to design and size a sustainable sanitation solution for the Ndiebene Gandiol 1 school located in the eponymous commune in northern Senegal. Field investigations led to the collection of wastewater samples. Their analysis revealed specific pollutant loads, including loads of BOD5 3.6966 kgO<sub>2</sub>/day and COD of 12.8775 kgO<sub>2</sub>/day, which were central to the design phase. Following a rigorous assessment of the existing sanitation infrastructure, constructed wetland (CWs) emerged as the most appropriate ecological solution. This system, valued for its ability to effectively remove contaminants, was tailored to the specific needs of the site. Consequently, the final design of the filter extends over 217.16 m<sup>2</sup>, divided into two cells of 108.58 m<sup>2</sup> each, with dimensions of 12.77 m in length and 8.5 m in width. The depth of the filtering medium is approximately 0.60 m, meeting the standards while ensuring maximized purification. Typha, an indigenous and prolific plant known for its purification abilities, was selected as the filtering agent. Concurrently, non-crushed gravel was chosen for its proven filtration capacity. This study is the result of a combination of scientific rigor and design expertise. It provides a holistic view of sanitation for Ndiebene Gandiol. The technical specifications and dimensions of the constructed wetland filter embody an approach that marries indepth analysis and practical application, all aimed at delivering an effective and long-lasting solution to the local sanitation challenges. By integrating precise scientific data with sanitation design expertise, this study delivers a holistic solution for Ndiebene Gandiol. The detailed dimensions and specifications of the constructed wetland filter reflect a methodology that combines meticulous analysis with practical adaptation, aiming to provide an effective and sustainable response to the challenges of rural and school sanitation in the northern region of Senegal.
基金the National Natural Science Foundation of China(project code:52202470)Jilin Province Natural Science Foundation(project codes:20220101205JC,20220101212JC)+2 种基金Jilin Province Specific Project of Industrial Technology Research&Development(project code:2020C025-2)2021 Interdisciplinary Integration and Innovation Project of Jilin University(project code:XJRCYB07)Free Exploration Project of Changsha Automotive Innovation Research Institute of Jilin University(project code:CAIRIZT20220202)。
文摘For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based species(N—C)/NOx is optimized using the Non-dominated Sorting Genetic Algorithm II(NSGA-II)with 200 generations.The optimized mechanism(named as 937b)is validated against combustion characteristics of ammonia/methane(which is used to examine the accuracy of N—C interactions)and ammonia/diesel blends.The ignition delay times(IDTs),the laminar flame speeds and most of key intermediate species during the combustion of ammonia/methane blends can be accurately simulated by 937b under a wide range of conditions.As for ammonia/diesel blends with various diesel energy fractions,reasonable predictions on the IDTs under pressures from 1.0 MPa to5.0 MPa as well as the laminar flame speeds are also achieved by 937b.In particular,with regard to the IDT simulations of ammonia/diesel blends,937b makes progress in both aspects of overall accuracy and computational efficiency,compared to a detailed ammonia/diesel mechanism.Further kinetic analysis reveals that the reaction pathway of ammonia during the combustion of ammonia/diesel blend mainly differs in the tendencies of oxygen additions to NH_2 and NH with different equivalence ratios.
基金Financial support from Ministerio de Ciencia e Innovación through projects PID2022-140143OB-I00(MCIN/AEI/10.13039/501100011033)and SO-CEX2019-000925-S(MCIN/AEI/10.13039/5011000110)supported by Marie Sk?odowska-Curie Actions Individual Fellowship grant funding to AMB,grant 101031365-SolTIMEthe support from the MSCA-COFUND I2:ICIQ Impulsion(GA 801474)。
文摘For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.
基金supported by the National Natural Science Foundation of China(22108238,21878259)the Zhejiang Provincial Natural Science Foundation of China(LR18B060001)+5 种基金Anhui Provincial Natural Science Founda-tion(1908085QB68)the Natural Science Foundation of the Anhui Higher Education Institutions of China(KJ2020A0275)Major Science and Technology Project of Anhui Province(201903a05020055)Foundation of Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology(ZJKL-ACEMT-1802)China Postdoctoral Science Foundation(2019M662060,2020T130580)Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology(BM2012110).
文摘The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.
基金supported by the National Natural Science Foundation of China(Grant Nos.42150710532 and 42103048).
文摘The knowledge of the residence time of formation water is fundamental to understanding the subsurface flow and hydrological setting.To better identify the origin and evolution of coal seam water and its impact on gas storage and production,this study collected coalbed methane co-produced water in the southeast Qinshui Basin and detected chemical and isotopic compositions,especially 36Cl and 129I concentrations.The calculated tracer ages of 129I(5.2–50.6 Ma)and 36Cl(0.13–0.76 Ma)are significantly younger than the age of coal-bearing formation(Pennsylvanian-Cisuralian),indicating freshwater recharge after coal deposition.The model that utilises 129I/I and 36Cl/Cl ratios to constrain the timing of recharge and the proportion of recharge water reveals that over 60%of pre-anthropogenic meteoric water entered coal seams since 10 Ma and mixed with residue initial deposition water,corresponding to the basin inversion in Cenozoic.The spatial distribution of major ion concentrations reveals the primary recharge pathway for meteoric water from coal outcrops at the eastern margin to the basin center.This study demonstrates the occurrence of higher gas production rates from wells that accept water recharge in recent times and suggests the possible potential of the non-stagnant zones for high gas production.
基金the financial support from the National Natural Science Foundation of China(52002146).
文摘Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon emissions.Renewables-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen production.Conventional water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen species.By virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas safely.Decoupled electrolysis has accelerated the development ofwater electrolysis technology for H_(2) production.However,itis still lack of a comprehensive and in-depth review in this field based on different types of RMs.This review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past decade.Several representative examples are then dis-played in detail according to the differences in the RMs.The rational choice and design of RMs have also been emphasized.Subsequently,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial photosynthesis.Finally,thekey characteristics and disadvantages of each type of mediator are sum-marized in depth.In addition,we present an outlook for future directions in decoupled water splitting.Thus,the flexibility in the design of mediators provides huge space for improving this electrochemical technology.@2024 Science Press and Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by ELSEVIER B.V.and Science Press.All rights reserved.
基金Under the auspices of Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA28020503,XDA23100102)National Key Research and Development Program of China(No.2019YFA0607101)+1 种基金Project of China Geological Survey(No.DD20230505)Excellent Scientific Research and Innovation Team of Universities in Anhui Province(No.2023AH010071)。
文摘As a typical region with high water demand for agricultural production,understanding the spatiotemporal surface water changes in Northeast China is critical for water resources management and sustainable development.However,the long-term variation characteristics of surface water of different water body types in Northeast China remain rarely explored.This study investigated how surface water bodies of different types(e.g.,lake,reservoir,river,coastal aquaculture,marsh wetland,ephemeral water) changed during1999–2020 in Northeast China based on various remote sensing-based datasets.The results showed that surface water in Northeast China grew dramatically in the past two decades,with an equivalent area increasing from 24 394 km^(2) in 1999 to 34 595 km^(2) in 2020.The surge of ephemeral water is the primary driver of surface water expansion,which could ascribe to shifted precipitation pattern.Marsh wetlands,rivers,and reservoirs experienced a similar trend,with an approximate 20% increase at the interdecadal scale.By contrast,coastal aquacultures and natural lakes remain relatively stable.This study is expected to provide a more comprehensive investigation of the surface water variability in Northeast China and has important practical significance for the scientific management of different types of surface water.
基金Under the auspices of National Natural Science Foundation of China(No.42201302)‘Double First-Class’University Construction Project of Lanzhou University(No.561120213)。
文摘Virtual water trade(VWT)provides a new perspective for alleviating water crisis and has thus attracted widespread attention.However,the heterogeneity of virtual water trade inside and outside the river basin and its influencing factors remains further study.In this study,for better investigating the pattern and heterogeneity of virtual water trade inside and outside provincial regions along the Yellow River Basin in 2015 using the input-output model(MRIO),we proposed two new concepts,i.e.,virtual water surplus and virtual water deficit,and then used the Logarithmic Mean Divisia Index(LMDI)model to identify the inherent mechanism of the imbalance of virtual water trade between provincial regions along the Yellow River Basin and the other four regions in China.The results show that:1)in provincial regions along the Yellow River Basin,the less developed the economy was,the larger the contribution of the agricultural sector in virtual water trade,while the smaller the contribution of the industrial sector.2)Due to the large output of agricultural products,the upstream and midstream provincial regions of the Yellow River Basin had a virtual water surplus,with a net outflow of virtual water of 2.7×10^(8) m^(3) and 0.9×10^(8) m^(3),respectively.3)provincial regions along the Yellow River Basin were in a virtual water deficit with the rest of China,and the decisive factor was the active degree of trade with the outside.This study would be beneficial to illuminate the trade-related water use issues in provincial regions along the Yellow River Basin,which has farreaching practical signific-ance for alleviating water scarcity.
基金supported by the National Natural Science Foundation of China[Nos.U21A20332,52103226,52202275,52203314,and 12204253]the Distinguished Young Scholars Fund of Jiangsu Province[No.BK20220061]the Fellowship of China Postdoctoral Science Foundation[No.2021M702382]。
文摘Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.
基金the Science and Engineering Research Board(SERB),Government of India for funding this work(Sanction No.EEQ/2021/001116)。
文摘The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.
基金supported by the research program funded by the TKG Huchemssupported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)granted financial resources from the Ministry of Trade,Industry&Energy,Republic of Korea(20213030040590)supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(2021R1A5A1028138)。
文摘Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and is regarded as a future technology for production of CO_(2)-free pure hydrogen.Herein,a heterostructural Pt-Ir dual-layer electrode is developed and shown to achieve successful long-term operation in an ammonia electrolyzer with an anion exchange membrane(AEM).This electrolyzer consisted of eight membra ne electrode assemblies(MEAs)with a total geometric area of 200 cm~2 on the anode side,which resulted in a hydrogen production rate of 25 L h~(-1).We observed the degradation in MEA performance attributed to changes in the anode catalyst layer during hydrogen production via ammonia electrolysis.Furthermore,we demonstrated the relationship between the ammonia oxidation reaction(AOR)and the oxygen evolution reaction(OER).