Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spect...Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.展开更多
Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such ...Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.展开更多
Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,a...Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,achieving high energy density in Zn||MnO_(2)batteries remains challenging,highlighting the need to understand the electrochemical reaction mechanisms underlying these batteries more deeply and optimize battery components,including electrodes and electrolytes.This review comprehensively summarizes the latest advancements for understanding the electrochemistry reaction mechanisms and designing electrodes and electrolytes for Zn||MnO_(2)batteries in mildly and strongly acidic environments.Furthermore,we highlight the key challenges hindering the extensive application of Zn||MnO_(2)batteries,including high-voltage requirements and areal capacity,and propose innovative solutions to overcome these challenges.We suggest that MnO_(2)/Mn^(2+)conversion in neutral electrolytes is a crucial aspect that needs to be addressed to achieve high-performance Zn||MnO_(2)batteries.These approaches could lead to breakthroughs in the future development of Zn||MnO_(2)batteries,off ering a more sustainable,costeff ective,and high-performance alternative to traditional batteries.展开更多
Economical water electrolysis requires highly active non-noble electrocatalysts to overcome the sluggish kinetics of the two half-cell reactions,oxygen evolution reaction,and hydrogen evolution reaction.Although inten...Economical water electrolysis requires highly active non-noble electrocatalysts to overcome the sluggish kinetics of the two half-cell reactions,oxygen evolution reaction,and hydrogen evolution reaction.Although intensive efforts have been committed to achieve a hydrogen economy,the expensive noble metal-based catalysts remain under consideration.Therefore,the engineering of self-supported electrocatalysts prepared using a direct growth strategy on three-dimensional(3D)nickel foam(NF)as a conductive substrate has garnered significant interest.This is due to the large active surface area and 3D porous network offered by these electrocatalysts,which can enhance the synergistic eff ect between the catalyst and the substrate,as well as improve electrocatalytic performance.Hydrothermal-assisted growth,microwave heating,electrodeposition,and other physical methods(i.e.,chemical vapor deposition and plasma treatment)have been applied to NF to fabricate competitive electrocatalysts with low overpotential and high stability.In this review,recent advancements in the development of self-supported electrocatalysts on 3D NF are described.Finally,we provide future perspectives of self-supported electrode platforms in electrochemical water splitting.展开更多
CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS acti...CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.展开更多
The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibite...The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibited similar phase compositions, specific surface areas, and Pt contents. High-resolution transmission electron microscopy coupled with pulsed CO adsorption revealed increased dispersity when photoreduction and the hydroxonitrate complex (Me _(4) N) _(2) [Pt _(2) (OH) _(2) (NO _(3) ) _(8) ] were used. The sample featured a high content of single-atom species and subnano-sized Pt clusters. The X-ray photoelectron spectroscopy results showed that the photoreduction method facilitated the appearance of a larger number of Pt ^(2+) states, which appeared owing to the strong metal-support interaction (SMSI) eff ect of the transfer of electron density from the electron-saturated defects on the TiO _(2) surface to Pt ^(4+) . In the hydrogen evolution reaction, samples with a significant fraction of the Pt ^(2+) ionic component, capable of generating short-lived Pt^(0) single-atom sites under irradiation due to the SMSI eff ect, exhibited the highest photocatalytic activity. The 0.5Pt(C)/TiO_(2) -Ph sample exhibited the highest hydrogen yield with a quantum efficiency of 0.53, retaining its activity even after 8 h of operation.展开更多
PPMG-based composite electrolytes were fabricated via the solution method using the polyvinyl alcohol and polyvinylpyrrolidone blend reinforced with various contents of sulfonated inorganic filler.Sulfuric acid was em...PPMG-based composite electrolytes were fabricated via the solution method using the polyvinyl alcohol and polyvinylpyrrolidone blend reinforced with various contents of sulfonated inorganic filler.Sulfuric acid was employed as the sulfonating agent to functionalize the external surface of the inorganic filler,i.e.,graphene oxide.The proton conductivities of the newly prepared proton exchange membranes(PEMs)were increased by increasing the temperature and content of sulfonated graphene oxide(SGO),i.e.,ranging from 0.025 S/cm to 0.060 S/cm.The induction of the optimum level of SGO is determined to be an excellent route to enhance ionic conductivity.The single-cell performance test was conducted by sandwiching the newly prepared PEMs between an anode(0.2 mg/cm^(2) Pt/Ru)and a cathode(0.2 mg/cm^(2) Pt)to prepare membrane electrode assemblies,followed by hot pressing under a pressure of approximately 100 kg/cm^(2) at 60℃for 5–10 min.The highest power densities achieved with PPMG PEMs were 14.9 and 35.60 mW/cm^(2) at 25℃and 70℃,respectively,at ambient pressure with 100%relative humidity.Results showed that the newly prepared PEMs exhibit good electrochemical performance.The results indicated that the prepared composite membrane with 6 wt%filler can be used as an alternative membrane for applications of high-performance proton exchange membrane fuel cell.展开更多
Molecular engineering is a crucial strategy for improving the photovoltaic performance of dye-sensitized solar cells(DSSCs). Despite the common use of the donor-π bridge-acceptor architecture in designing sensitizers...Molecular engineering is a crucial strategy for improving the photovoltaic performance of dye-sensitized solar cells(DSSCs). Despite the common use of the donor-π bridge-acceptor architecture in designing sensitizers, the underlying structure-performance relationship remains not fully understood. In this study, we synthesized and characterized three sensitizers: MOTP-Pyc, MOS_(2)P-Pyc, and MOTS_(2)P-Pyc, all featuring a bipyrimidine acceptor. Absorption spectra, cyclic voltammetry, and transient photoluminescence spectra reveal a photo-induced electron transfer(PET) process in the excited sensitizers. Electron spin resonance spectroscopy confirmed the presence of charge-separated states. The varying donor and π-bridge structures among the three sensitizers led to differences in their conjugation effect, influencing light absorption abilities and PET processes and ultimately impacting the photovoltaic performance. Among the synthesized sensitizers, MOTP-Pyc demonstrated a DSSC efficiency of 3.04%. Introducing an additional thienothiophene block into the π-bridge improved the DSSC efficiency to 4.47% for MOTS_(2)P-Pyc. Conversely, replacing the phenyl group with a thienothiophene block reduced DSSC efficiency to 2.14% for MOS_(2)P-Pyc. Given the proton-accepting ability of the bipyrimidine module, we treated the dye-sensitized TiO_(2) photoanodes with hydroiodic acid(HI), significantly broadening the light absorption range. This treatment greatly enhanced the short-circuit current density of DSSCs owing to the enhanced electron-withdrawing ability of the acceptor. Consequently, the HI-treated MOTS_(2)P-Pyc-based DSSCs achieved the highest power conversion efficiency of 7.12%, comparable to that of the N719 dye at 7.09%. This work reveals the positive role of bipyrimidine in the design of organic sensitizers for DSSC applications.展开更多
In recent times, lithium-ion batteries have been widely used owing to their high energy density, extended cycle lifespan, and minimal self-discharge rate. The design of high-speed rechargeable lithium-ion batteries fa...In recent times, lithium-ion batteries have been widely used owing to their high energy density, extended cycle lifespan, and minimal self-discharge rate. The design of high-speed rechargeable lithium-ion batteries faces a significant challenge owing to the need to increase average electric power during charging. This challenge results from the direct influence of the power level on the rate of chemical reactions occurring in the battery electrodes. In this study, the Taguchi optimization method was used to enhance the average electric power during the charging process of lithium-ion batteries. The Taguchi technique is a statistical strategy that facilitates the systematic and efficient evaluation of numerous experimental variables. The proposed method involved varying seven input factors, including positive electrode thickness, positive electrode material, positive electrode active material volume fraction, negative electrode active material volume fraction, separator thickness, positive current collector thickness, and negative current collector thickness. Three levels were assigned to each control factor to identify the optimal conditions and maximize the average electric power during charging. Moreover, a variance assessment analysis was conducted to validate the results obtained from the Taguchi analysis. The results revealed that the Taguchi method was an eff ective approach for optimizing the average electric power during the charging of lithium-ion batteries. This indicates that the positive electrode material, followed by the separator thickness and the negative electrode active material volume fraction, was key factors significantly infl uencing the average electric power during the charging of lithium-ion batteries response. The identification of optimal conditions resulted in the improved performance of lithium-ion batteries, extending their potential in various applications. Particularly, lithium-ion batteries with average electric power of 16 W and 17 W during charging were designed and simulated in the range of 0-12000 s using COMSOL Multiphysics software. This study efficiently employs the Taguchi optimization technique to develop lithium-ion batteries capable of storing a predetermined average electric power during the charging phase. Therefore, this method enables the battery to achieve complete charging within a specific timeframe tailored to a specificapplication. The implementation of this method can save costs, time, and materials compared with other alternative methods, such as the trial-and-error approach.展开更多
We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x )catalysts(RuO_(2)/CoMo_...We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x )catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance( η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment.展开更多
Non-precious metal electrocatalysts(such as Fe-N-C materials) for the oxygen(O_(2)) reduction reaction demand a high catalyst loading in fuel cell devices to achieve workable performance. However, the extremely low so...Non-precious metal electrocatalysts(such as Fe-N-C materials) for the oxygen(O_(2)) reduction reaction demand a high catalyst loading in fuel cell devices to achieve workable performance. However, the extremely low solubility of O_(2) in water creates severe mass transport resistance in the thick catalyst layer of Fe-N-C catalysts. Here, we introduce silicalite-1 nanocrystals with hydrophobic cavities as sustainable O_(2) reservoirs to overcome the mass transport issue of Fe-N-C catalysts. The extra O_(2) supply to the adjacent catalysts significantly alleviated the negative effects of the severe mass transport resistance. The hybrid catalyst(Fe-N-C@silicalite-1) achieved a higher limiting current density than Fe-N-C in the half-cell test. In the H_(2)-O_(2) and H_2-air proton exchange membrane fuel cells, Fe-N-C@silicalite-1 exhibited a 16.3% and 20.2% increase in peak power density compared with Fe-N-C, respectively. The O_(2)-concentrating additive provides an effective approach for improving the mass transport imposed by the low solubility of O_(2) in water.展开更多
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ...N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.展开更多
Because of the low reactivity of cyclic nitrides,liquid-phase synthesis of carbon nitride introduces challenges despite its favorable potential for energy-efficient preparation and superior applications.In this study,...Because of the low reactivity of cyclic nitrides,liquid-phase synthesis of carbon nitride introduces challenges despite its favorable potential for energy-efficient preparation and superior applications.In this study,we demonstrate a strong interaction between citric acid and melamine through experimental observation and theoretical simulation,which eff ectively activates melamine-condensation activity and produces carbon-rich carbon nitride nanosheets(CCN NSs)during hydrothermal reaction.Under a large specific surface area and increased light absorption,these CCN NSs demonstrate significantly enhanced photocatalytic activity in CO_(2) reduction,increasing the CO production rate by approximately tenfold compared with hexagonal melamine(h-Me).Moreover,the product selectivity of CCN NSs reaches up to 93.5%to generate CO from CO_(2).Furthermore,the annealed CCN NSs exhibit a CO conversion rate of up to 95.30μmol/(g h),which indicates an 18-fold increase compared with traditional carbon nitride.During the CCN NS synthesis,nitrogen-doped carbon quantum dots(NDC QDs)are simultaneously produced and remain suspended in the supernatant after centrifugation.These QDs disperse well in water and exhibit excellent luminescent properties(QY=67.2%),allowing their application in the design of selective and sensitive sensors to detect pollutants such as pesticide 2,4-dichlorophenol with a detection limit of as low as 0.04μmol/L.Notably,the simultaneous synthesis of CCN NSs and NDC QDs provides a cost-eff ective and highly efficient process,yielding products with superior capabilities for catalytic conversion of CO_(2) and pollutant detection,respectively.展开更多
The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation...The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation technique to fabricate nitrogen(N)and chlorine(Cl)co-doped graphene nanosheets(i.e.,N-Cl-G)via the application of constant voltage on graphite in a mixture of 0.1 mol/L H_(2)SO_(4)and 0.1 mol/L NH_(4)Cl without using dangerous and exhaustive operation.The introduction of Cl(with its large radius)and N,both with high electrical negativity,facilitates the modulation of the electronic structure of graphene and creation of rich structural defects in it.Consequently,in the as-constructed supercapacitors,N-Cl-G exhibits a high specific capacitance of 77 F/g at 0.2 A/g and remarkable cycling stability with 91.7%retention of initial capacitance after 20,000 cycles at 10 A/g.Furthermore,a symmetrical supercapacitor assembled with N-Cl-G as the positive and negative electrodes(denoted as N-Cl-G//N-Cl-G)exhibits an energy density of 3.38 Wh/kg at a power density of 600 W/kg and superior cycling stability with almost no capacitance loss after 5000 cycles at 5 A/g.This study provides a scalable protocol for the facile fabrication of high-performance co-doped graphene as an electrode material candidate for supercapacitors.展开更多
Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose...Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose technology uses an array of sensors to detect and quantify gases, including CO_(2), in the air. This study briefly introduces the concept of eNose technology and potential applications thereof in monitoring CO_(2) conversion processes. It also provides background information on biological CO_(2) conversion processes. Furthermore, the working principles of eNose technology vis-à-vis gas detection are discussed along with its advantages and limitations versus traditional monitoring methods. This study also provides case studies that have used this technology for monitoring biological CO_(2) conversion processes. eNose-predicted measurements were observed to be completely aligned with biological parameters for R~2 values of 0.864, 0.808, 0.802, and 0.948. We test eNose technology in a variety of biological settings, such as algae farms or bioreactors, to determine its effectiveness in monitoring CO_(2) conversion processes. We also explore the potential benefits of employing this technology vis-à-vis monitoring biological CO_(2) conversion processes, such as increased reaction efficiency and reduced costs versus traditional monitoring methods. Moreover, future directions and challenges of using this technology in CO_(2) capture and conversion have been discussed. Overall, we believe this study would contribute to developing new and innovative methods for monitoring biological CO_(2) conversion processes and mitigating climate change.展开更多
All-solid-state lithium-metal batteries(ASSLMBs)are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features.Among various solid electrolytes,s...All-solid-state lithium-metal batteries(ASSLMBs)are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features.Among various solid electrolytes,sulfide solid electrolyte(SSE)Li_(6)PS_(5)Cl has garnered significant attention.However,its application is limited by its poor cyclability and low critical current density(CCD).In this study,we introduce a novel approach to enhance the performance of Li_(6)PS_(5)Cl by doping it with fluorine,using lithium fluoride nanoparticles(LiFs)as the doping precursor.The F-doped electrolyte Li_(6)PS_(5)Cl-0.2LiF(nano)shows a doubled CCD,from 0.5 to 1.0 mA/cm^(2) without compromising the ionic conductivity;in fact,conductivity is enhanced from 2.82 to 3.30 mS/cm,contrary to the typical performance decline seen in conventionally doped Li_(6)PS_(5)Cl electrolytes.In symmetric Li|SSE|Li cells,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is 4 times longer than that of Li_(6)PS_(5)Cl,achieving 1500 h vs.371 h under a charging/discharging current density of 0.2 mA/cm^(2).In Li|SSE|LiNbO_(3)@NCM721 full cells,which are tested under a cycling rate of 0.1 C at 30℃,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is four times that of Li_(6)PS_(5)Cl,reaching 100 cycles vs.26 cycles.Therefore,the doping of nano-LiF off ers a promising approach to developing high-performance Li_(6)PS_(5)Cl for ASSLMBs.展开更多
With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions ...With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.展开更多
Recently,electronic skins and fl exible wearable devices have been developed for widespread applications in medical monitoring,artifi cial intelligence,human–machine interaction,and artifi cial prosthetics.Flexible p...Recently,electronic skins and fl exible wearable devices have been developed for widespread applications in medical monitoring,artifi cial intelligence,human–machine interaction,and artifi cial prosthetics.Flexible proximity sensors can accurately perceive external objects without contact,introducing a new way to achieve an ultrasensitive perception of objects.This article reviews the progress of fl exible capacitive proximity sensors,fl exible triboelectric proximity sensors,and fl exible gate-enhanced proximity sensors,focusing on their applications in the electronic skin fi eld.Herein,their working mechanism,materials,preparation methods,and research progress are discussed in detail.Finally,we summarize the future challenges in developing fl exible proximity sensors.展开更多
The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it rem...The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major challenge.While density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses limitations.This paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex systems.Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and selectivity.We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms.The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production.We confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR activity.Our developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other systems.This work provides insights into the low-cost and rational design of high-performance SACs.展开更多
Energy for space vehicles in low Earth orbit(LEO) is mainly generated by solar arrays, and the service time of the vehicles is controlled by the lifetime of these arrays, which depends mainly on the lifetime of the in...Energy for space vehicles in low Earth orbit(LEO) is mainly generated by solar arrays, and the service time of the vehicles is controlled by the lifetime of these arrays, which depends mainly on the lifetime of the interconnects. To increase the service life of LEO satellites, molybdenum/platinum/silver(Mo/Pt/Ag) laminated metal matrix composite(LMMC) interconnectors are widely used in place of Mo/Ag LMMC and Ag interconnectors in solar arrays. A 2D thermal-electrical-mechanical coupled axisymmetric model was established to simulate the behavior of the parallel gap resistance welding(PGRW) process for solar cells and Mo/Pt/Ag composite interconnectors using the commercial software ANSYS. The direct multicoupled PLANE223 element and the contact pair elements TARGE169 and CONTA172 were employed. A transitional meshing method was applied to solve the meshing problem due to the ultrathin(1 μm) intermediate Pt layer. A comparison of the analysis results with the experimental results revealed that the best parameters were 60 W, 60 ms, and 0.0138 MPa. The voltage and current predicted by the finite element method agreed well with the experimental results. This study contributes to a further understanding of the mechanism of PGRW and provides guidance for finite element simulation of the process of welding with an ultrathin interlayer.展开更多
基金supported by Russian Science Foundation (No.#21-73-10235)
文摘Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.
基金the financial support from by the National Key Research and Development Program of China(No.2022YFB4101800)National Natural Science Foundation of China(No.22278298)Program for Introducing Talents of Discipline to Universities of China(No.BP0618007).
文摘Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.
文摘Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,achieving high energy density in Zn||MnO_(2)batteries remains challenging,highlighting the need to understand the electrochemical reaction mechanisms underlying these batteries more deeply and optimize battery components,including electrodes and electrolytes.This review comprehensively summarizes the latest advancements for understanding the electrochemistry reaction mechanisms and designing electrodes and electrolytes for Zn||MnO_(2)batteries in mildly and strongly acidic environments.Furthermore,we highlight the key challenges hindering the extensive application of Zn||MnO_(2)batteries,including high-voltage requirements and areal capacity,and propose innovative solutions to overcome these challenges.We suggest that MnO_(2)/Mn^(2+)conversion in neutral electrolytes is a crucial aspect that needs to be addressed to achieve high-performance Zn||MnO_(2)batteries.These approaches could lead to breakthroughs in the future development of Zn||MnO_(2)batteries,off ering a more sustainable,costeff ective,and high-performance alternative to traditional batteries.
基金supported by The Chinese Academy of Sciences (CAS) President’s International Fellowship Initiative (No. 2023VCB0014)The National Natural Science Foundation of China (No. 52203284)Shenzhen Science and Technology Program (Nos. GJHZ20220913143801003 and RCBS20221008093057026)
文摘Economical water electrolysis requires highly active non-noble electrocatalysts to overcome the sluggish kinetics of the two half-cell reactions,oxygen evolution reaction,and hydrogen evolution reaction.Although intensive efforts have been committed to achieve a hydrogen economy,the expensive noble metal-based catalysts remain under consideration.Therefore,the engineering of self-supported electrocatalysts prepared using a direct growth strategy on three-dimensional(3D)nickel foam(NF)as a conductive substrate has garnered significant interest.This is due to the large active surface area and 3D porous network offered by these electrocatalysts,which can enhance the synergistic eff ect between the catalyst and the substrate,as well as improve electrocatalytic performance.Hydrothermal-assisted growth,microwave heating,electrodeposition,and other physical methods(i.e.,chemical vapor deposition and plasma treatment)have been applied to NF to fabricate competitive electrocatalysts with low overpotential and high stability.In this review,recent advancements in the development of self-supported electrocatalysts on 3D NF are described.Finally,we provide future perspectives of self-supported electrode platforms in electrochemical water splitting.
基金The research was carried out within the State Assignment of the Ministry of Science and Higher Education of the Russian Federation(project No.FFUG-2024-0036)。
文摘CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.
文摘The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibited similar phase compositions, specific surface areas, and Pt contents. High-resolution transmission electron microscopy coupled with pulsed CO adsorption revealed increased dispersity when photoreduction and the hydroxonitrate complex (Me _(4) N) _(2) [Pt _(2) (OH) _(2) (NO _(3) ) _(8) ] were used. The sample featured a high content of single-atom species and subnano-sized Pt clusters. The X-ray photoelectron spectroscopy results showed that the photoreduction method facilitated the appearance of a larger number of Pt ^(2+) states, which appeared owing to the strong metal-support interaction (SMSI) eff ect of the transfer of electron density from the electron-saturated defects on the TiO _(2) surface to Pt ^(4+) . In the hydrogen evolution reaction, samples with a significant fraction of the Pt ^(2+) ionic component, capable of generating short-lived Pt^(0) single-atom sites under irradiation due to the SMSI eff ect, exhibited the highest photocatalytic activity. The 0.5Pt(C)/TiO_(2) -Ph sample exhibited the highest hydrogen yield with a quantum efficiency of 0.53, retaining its activity even after 8 h of operation.
文摘PPMG-based composite electrolytes were fabricated via the solution method using the polyvinyl alcohol and polyvinylpyrrolidone blend reinforced with various contents of sulfonated inorganic filler.Sulfuric acid was employed as the sulfonating agent to functionalize the external surface of the inorganic filler,i.e.,graphene oxide.The proton conductivities of the newly prepared proton exchange membranes(PEMs)were increased by increasing the temperature and content of sulfonated graphene oxide(SGO),i.e.,ranging from 0.025 S/cm to 0.060 S/cm.The induction of the optimum level of SGO is determined to be an excellent route to enhance ionic conductivity.The single-cell performance test was conducted by sandwiching the newly prepared PEMs between an anode(0.2 mg/cm^(2) Pt/Ru)and a cathode(0.2 mg/cm^(2) Pt)to prepare membrane electrode assemblies,followed by hot pressing under a pressure of approximately 100 kg/cm^(2) at 60℃for 5–10 min.The highest power densities achieved with PPMG PEMs were 14.9 and 35.60 mW/cm^(2) at 25℃and 70℃,respectively,at ambient pressure with 100%relative humidity.Results showed that the newly prepared PEMs exhibit good electrochemical performance.The results indicated that the prepared composite membrane with 6 wt%filler can be used as an alternative membrane for applications of high-performance proton exchange membrane fuel cell.
基金supported by the National Natural Science Foundation of China(Nos.21776207 and 21576195)。
文摘Molecular engineering is a crucial strategy for improving the photovoltaic performance of dye-sensitized solar cells(DSSCs). Despite the common use of the donor-π bridge-acceptor architecture in designing sensitizers, the underlying structure-performance relationship remains not fully understood. In this study, we synthesized and characterized three sensitizers: MOTP-Pyc, MOS_(2)P-Pyc, and MOTS_(2)P-Pyc, all featuring a bipyrimidine acceptor. Absorption spectra, cyclic voltammetry, and transient photoluminescence spectra reveal a photo-induced electron transfer(PET) process in the excited sensitizers. Electron spin resonance spectroscopy confirmed the presence of charge-separated states. The varying donor and π-bridge structures among the three sensitizers led to differences in their conjugation effect, influencing light absorption abilities and PET processes and ultimately impacting the photovoltaic performance. Among the synthesized sensitizers, MOTP-Pyc demonstrated a DSSC efficiency of 3.04%. Introducing an additional thienothiophene block into the π-bridge improved the DSSC efficiency to 4.47% for MOTS_(2)P-Pyc. Conversely, replacing the phenyl group with a thienothiophene block reduced DSSC efficiency to 2.14% for MOS_(2)P-Pyc. Given the proton-accepting ability of the bipyrimidine module, we treated the dye-sensitized TiO_(2) photoanodes with hydroiodic acid(HI), significantly broadening the light absorption range. This treatment greatly enhanced the short-circuit current density of DSSCs owing to the enhanced electron-withdrawing ability of the acceptor. Consequently, the HI-treated MOTS_(2)P-Pyc-based DSSCs achieved the highest power conversion efficiency of 7.12%, comparable to that of the N719 dye at 7.09%. This work reveals the positive role of bipyrimidine in the design of organic sensitizers for DSSC applications.
文摘In recent times, lithium-ion batteries have been widely used owing to their high energy density, extended cycle lifespan, and minimal self-discharge rate. The design of high-speed rechargeable lithium-ion batteries faces a significant challenge owing to the need to increase average electric power during charging. This challenge results from the direct influence of the power level on the rate of chemical reactions occurring in the battery electrodes. In this study, the Taguchi optimization method was used to enhance the average electric power during the charging process of lithium-ion batteries. The Taguchi technique is a statistical strategy that facilitates the systematic and efficient evaluation of numerous experimental variables. The proposed method involved varying seven input factors, including positive electrode thickness, positive electrode material, positive electrode active material volume fraction, negative electrode active material volume fraction, separator thickness, positive current collector thickness, and negative current collector thickness. Three levels were assigned to each control factor to identify the optimal conditions and maximize the average electric power during charging. Moreover, a variance assessment analysis was conducted to validate the results obtained from the Taguchi analysis. The results revealed that the Taguchi method was an eff ective approach for optimizing the average electric power during the charging of lithium-ion batteries. This indicates that the positive electrode material, followed by the separator thickness and the negative electrode active material volume fraction, was key factors significantly infl uencing the average electric power during the charging of lithium-ion batteries response. The identification of optimal conditions resulted in the improved performance of lithium-ion batteries, extending their potential in various applications. Particularly, lithium-ion batteries with average electric power of 16 W and 17 W during charging were designed and simulated in the range of 0-12000 s using COMSOL Multiphysics software. This study efficiently employs the Taguchi optimization technique to develop lithium-ion batteries capable of storing a predetermined average electric power during the charging phase. Therefore, this method enables the battery to achieve complete charging within a specific timeframe tailored to a specificapplication. The implementation of this method can save costs, time, and materials compared with other alternative methods, such as the trial-and-error approach.
基金supported by National Nature Science Foundation of China(22379106)Carbon Energy Technology Co.,Ltd.(0501001107)。
文摘We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x )catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance( η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment.
基金financially supported by the Natural Science Foundation of Beijing Municipality(No.Z200012)the National Natural Science Foundation of China(Nos.U21A20328 and 21975010)+2 种基金the National Key Research and Development Program of China(No. 2021YFB4000601)the China Postdoctoral Science Foundation(No.2022M720013)the Postdoctoral Fellowship Program of CPSF(No.GZB20230926)。
文摘Non-precious metal electrocatalysts(such as Fe-N-C materials) for the oxygen(O_(2)) reduction reaction demand a high catalyst loading in fuel cell devices to achieve workable performance. However, the extremely low solubility of O_(2) in water creates severe mass transport resistance in the thick catalyst layer of Fe-N-C catalysts. Here, we introduce silicalite-1 nanocrystals with hydrophobic cavities as sustainable O_(2) reservoirs to overcome the mass transport issue of Fe-N-C catalysts. The extra O_(2) supply to the adjacent catalysts significantly alleviated the negative effects of the severe mass transport resistance. The hybrid catalyst(Fe-N-C@silicalite-1) achieved a higher limiting current density than Fe-N-C in the half-cell test. In the H_(2)-O_(2) and H_2-air proton exchange membrane fuel cells, Fe-N-C@silicalite-1 exhibited a 16.3% and 20.2% increase in peak power density compared with Fe-N-C, respectively. The O_(2)-concentrating additive provides an effective approach for improving the mass transport imposed by the low solubility of O_(2) in water.
基金We acknowledge the National Natural Science Foundation of China(No.22275134)for fi nancial support.
文摘N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.
基金supported by the National High Technology Research and Development Program of China(No.2021YFF1200200)the Peiyang Talents Project of Tianjin University。
文摘Because of the low reactivity of cyclic nitrides,liquid-phase synthesis of carbon nitride introduces challenges despite its favorable potential for energy-efficient preparation and superior applications.In this study,we demonstrate a strong interaction between citric acid and melamine through experimental observation and theoretical simulation,which eff ectively activates melamine-condensation activity and produces carbon-rich carbon nitride nanosheets(CCN NSs)during hydrothermal reaction.Under a large specific surface area and increased light absorption,these CCN NSs demonstrate significantly enhanced photocatalytic activity in CO_(2) reduction,increasing the CO production rate by approximately tenfold compared with hexagonal melamine(h-Me).Moreover,the product selectivity of CCN NSs reaches up to 93.5%to generate CO from CO_(2).Furthermore,the annealed CCN NSs exhibit a CO conversion rate of up to 95.30μmol/(g h),which indicates an 18-fold increase compared with traditional carbon nitride.During the CCN NS synthesis,nitrogen-doped carbon quantum dots(NDC QDs)are simultaneously produced and remain suspended in the supernatant after centrifugation.These QDs disperse well in water and exhibit excellent luminescent properties(QY=67.2%),allowing their application in the design of selective and sensitive sensors to detect pollutants such as pesticide 2,4-dichlorophenol with a detection limit of as low as 0.04μmol/L.Notably,the simultaneous synthesis of CCN NSs and NDC QDs provides a cost-eff ective and highly efficient process,yielding products with superior capabilities for catalytic conversion of CO_(2) and pollutant detection,respectively.
基金supported by National Science Foundation of China(No.52201254)Natural Science Foundation of Shandong Province(Nos.ZR2020MB090,ZR2020MB027,and ZR2020QE012)+1 种基金the project of“20 Items of University”of Jinan(No.202228046)the Taishan Scholar Project of Shandong Province(No.tsqn202306226)。
文摘The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation technique to fabricate nitrogen(N)and chlorine(Cl)co-doped graphene nanosheets(i.e.,N-Cl-G)via the application of constant voltage on graphite in a mixture of 0.1 mol/L H_(2)SO_(4)and 0.1 mol/L NH_(4)Cl without using dangerous and exhaustive operation.The introduction of Cl(with its large radius)and N,both with high electrical negativity,facilitates the modulation of the electronic structure of graphene and creation of rich structural defects in it.Consequently,in the as-constructed supercapacitors,N-Cl-G exhibits a high specific capacitance of 77 F/g at 0.2 A/g and remarkable cycling stability with 91.7%retention of initial capacitance after 20,000 cycles at 10 A/g.Furthermore,a symmetrical supercapacitor assembled with N-Cl-G as the positive and negative electrodes(denoted as N-Cl-G//N-Cl-G)exhibits an energy density of 3.38 Wh/kg at a power density of 600 W/kg and superior cycling stability with almost no capacitance loss after 5000 cycles at 5 A/g.This study provides a scalable protocol for the facile fabrication of high-performance co-doped graphene as an electrode material candidate for supercapacitors.
基金supported by the National Key Technologies R & D Program of China during the 14th Five-Year Plan period (No. 2021YFD1700904)Henan Provincial Important Project (No. 221100320200)+1 种基金State Key Laboratory of Wheat and Maize Crap Science (No. SKL2023ZZ09)the Henan Center for Outstanding Overseas Scientists (No. GZS2021007)。
文摘Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose technology uses an array of sensors to detect and quantify gases, including CO_(2), in the air. This study briefly introduces the concept of eNose technology and potential applications thereof in monitoring CO_(2) conversion processes. It also provides background information on biological CO_(2) conversion processes. Furthermore, the working principles of eNose technology vis-à-vis gas detection are discussed along with its advantages and limitations versus traditional monitoring methods. This study also provides case studies that have used this technology for monitoring biological CO_(2) conversion processes. eNose-predicted measurements were observed to be completely aligned with biological parameters for R~2 values of 0.864, 0.808, 0.802, and 0.948. We test eNose technology in a variety of biological settings, such as algae farms or bioreactors, to determine its effectiveness in monitoring CO_(2) conversion processes. We also explore the potential benefits of employing this technology vis-à-vis monitoring biological CO_(2) conversion processes, such as increased reaction efficiency and reduced costs versus traditional monitoring methods. Moreover, future directions and challenges of using this technology in CO_(2) capture and conversion have been discussed. Overall, we believe this study would contribute to developing new and innovative methods for monitoring biological CO_(2) conversion processes and mitigating climate change.
基金supported by the National Key Research and Development Program of China(No.2018YFE0111600)the Haihe Laboratory of Sustainable Chemical Transformations(No.CYZC202307)for financial support。
文摘All-solid-state lithium-metal batteries(ASSLMBs)are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features.Among various solid electrolytes,sulfide solid electrolyte(SSE)Li_(6)PS_(5)Cl has garnered significant attention.However,its application is limited by its poor cyclability and low critical current density(CCD).In this study,we introduce a novel approach to enhance the performance of Li_(6)PS_(5)Cl by doping it with fluorine,using lithium fluoride nanoparticles(LiFs)as the doping precursor.The F-doped electrolyte Li_(6)PS_(5)Cl-0.2LiF(nano)shows a doubled CCD,from 0.5 to 1.0 mA/cm^(2) without compromising the ionic conductivity;in fact,conductivity is enhanced from 2.82 to 3.30 mS/cm,contrary to the typical performance decline seen in conventionally doped Li_(6)PS_(5)Cl electrolytes.In symmetric Li|SSE|Li cells,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is 4 times longer than that of Li_(6)PS_(5)Cl,achieving 1500 h vs.371 h under a charging/discharging current density of 0.2 mA/cm^(2).In Li|SSE|LiNbO_(3)@NCM721 full cells,which are tested under a cycling rate of 0.1 C at 30℃,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is four times that of Li_(6)PS_(5)Cl,reaching 100 cycles vs.26 cycles.Therefore,the doping of nano-LiF off ers a promising approach to developing high-performance Li_(6)PS_(5)Cl for ASSLMBs.
基金supported by the support by the Natural Science Foundation of China projects(Nos.22225604 and 22076082)the Frontiers Science Center for New Organic Matter(No.63181206)Haihe Laboratory of Sustainable Chemical Transformations.
文摘With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.
基金supported by the National Key R&D Program of China(Nos.2022 YFF 1202700 and 2022YFB3203500)National Natural Science Foundation of China(Nos.62225403,62375046,51973024,an d U19A2091)+2 种基金“111”Project(No.B13013)Natur al Sci ence Foundation of Jilin Pro vin ce(No.20230101113JC)the Funding from Jilin Pr ovince(No.20220502002GH).
文摘Recently,electronic skins and fl exible wearable devices have been developed for widespread applications in medical monitoring,artifi cial intelligence,human–machine interaction,and artifi cial prosthetics.Flexible proximity sensors can accurately perceive external objects without contact,introducing a new way to achieve an ultrasensitive perception of objects.This article reviews the progress of fl exible capacitive proximity sensors,fl exible triboelectric proximity sensors,and fl exible gate-enhanced proximity sensors,focusing on their applications in the electronic skin fi eld.Herein,their working mechanism,materials,preparation methods,and research progress are discussed in detail.Finally,we summarize the future challenges in developing fl exible proximity sensors.
基金the National Key R&D Program of China(No.2022YFE0102000)the National Natural Science Foundation of China(Nos.22121004,U22A20409,22250008,and 22108197)+2 种基金the Haihe Laboratory of Sustainable Chemical Transformations,the Natural Science Foundation of Tianjin City(No.21JCZXJC00060)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)the XPLORER PRIZE for financial support。
文摘The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major challenge.While density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses limitations.This paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex systems.Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and selectivity.We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms.The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production.We confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR activity.Our developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other systems.This work provides insights into the low-cost and rational design of high-performance SACs.
基金supported by the National Key Research and Development Program of China(Nos. 2018YFB0703904 and 2017YFE0302600)。
文摘Energy for space vehicles in low Earth orbit(LEO) is mainly generated by solar arrays, and the service time of the vehicles is controlled by the lifetime of these arrays, which depends mainly on the lifetime of the interconnects. To increase the service life of LEO satellites, molybdenum/platinum/silver(Mo/Pt/Ag) laminated metal matrix composite(LMMC) interconnectors are widely used in place of Mo/Ag LMMC and Ag interconnectors in solar arrays. A 2D thermal-electrical-mechanical coupled axisymmetric model was established to simulate the behavior of the parallel gap resistance welding(PGRW) process for solar cells and Mo/Pt/Ag composite interconnectors using the commercial software ANSYS. The direct multicoupled PLANE223 element and the contact pair elements TARGE169 and CONTA172 were employed. A transitional meshing method was applied to solve the meshing problem due to the ultrathin(1 μm) intermediate Pt layer. A comparison of the analysis results with the experimental results revealed that the best parameters were 60 W, 60 ms, and 0.0138 MPa. The voltage and current predicted by the finite element method agreed well with the experimental results. This study contributes to a further understanding of the mechanism of PGRW and provides guidance for finite element simulation of the process of welding with an ultrathin interlayer.