Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary ba...Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.展开更多
With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains a...With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.展开更多
The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxome...The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxometalate(POM)nanoclusters with high catalytic activity and cobalt selenide with strong polarity are initially complemented to construct a PMo_(12)/CoSe_(2)@NC/CNTs multifunctional separator that can simultaneously solve the above problems.A series of experimental and theoretical results demonstrate that the Keggin-type POM,H_(3)PMo_(12)O_(40)nH_(2)O(PMo_(12))nanoclusters could function as catalytic centers for sulfur-involved transformations,with the CoSe_(2)nanoparticles serving as adsorption sites for soluble polysulfides.Accordingly,the assembled battery with the PMo_(12)/CoSe_(2)@NC/CNTs modified separator achieves an initial discharge capacity of 1263.79 mA h g^(-1),maintaining 635.77 mA h g^(-1),with a capacity decay rate of 0.06%per cycle after 500 cycles at 3C.This work provides a strategic approach for incorporating POM nanoclusters with polar periodic nanomaterials in LSB separators,contributing to the development of multifunctional separator materials,thus promoting the advancement of energy storage systems.展开更多
Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic de...Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic devices.However,the performance of TMDs-based devices is hampered by the suboptimal quality of metal electrodes contacting the atomically thin TMDs layers.Understanding the mechanisms that influence contact quality is crucial for advancing TMDs devices.In this study,we investigated the conductive properties of tungsten selenide(WSe_(2))-based devices with different film thicknesses.Using the transmission line method,a negative correlation between contact resistance and film thickness in multi-electrode devices was revealed.Additionally,repeatability tests conducted at varied temperatures indicated enhanced device stability with increasing film thickness.Theoretical analysis,supported by thermionic emission theory and thermal simulations,suggests that the degradation in electrical properties is primarily due to the thermal effect at the contact interface.Furthermore,we found that van der Waals contacts could mitigate the thermal effect through a metal transfer method.Our findings elucidate the critical role of contact resistance in the electronic performance of 2D material-based field-effect transistors(FETs),which further expands their potential in the next generation of electronic and optoelectronic devices.展开更多
Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some diffic...Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some difficulties in exploring practical applications in which cycling stability and cycle life are awful owing to the shuttling effect of lithium polysulfides(LiPSs)and low sulfur utilization.In this work,by synthesizing Co_(3)Se_(4) nanoparticles onto N-doped carbon(NC)polyhedra interconnected with carbon nanotubes(CNTs),NC@Co_(3)Se_(4)/CNTs is proposed as a multifunctional sulfur carrier.The Co_(3)Se_(4) nanoparticles fleetly catalyze the conversion of LiPSs and availably immobilize LiPSs.Meanwhile,the NC polyhedral skeleton enhances the electronic conductivity of active sulfur,while the CNTs facilitate Li+diffusion and supply a mass of conductive channels.Density-functional theory(DFT)calculations demonstrate the relevant mechanisms.That is to say,the NC@Co_(3)Se_(4)/CNTs benefit from the synergistic effect of Co_(3)Se_(4) nanoparticles(highly catalytic ability and strong adsorbability for LiPSs)and the special carbonaceous structure,rapidly converting LiPSs and inhibiting the shuttle of LiPSs.Therefore,lithium-sulfur battery assembled with S/NC@Co_(3)Se_(4)/CNTs cathode as well as nitrogen and sulfur co-doped carbon-coated polypropylene(N,S-C/PP)separator possesses a high initial discharge capacity of 1413 mAh·g-1 at 0.12C and persistently circulates for 1000 cycles at 1C with a capacity attenuation rate per cycle of 0.034%.This work provides a realistic idea for the use of transition metal selenide in the field of high-performance LSBs.展开更多
Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense...Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.展开更多
Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrent...Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.展开更多
Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a t...Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a trimetallic nickel–magnesium-manganese selenide(NMMSe)electrode with a well-defined nanosphere morphology was prepared using a low-cost and rapid electrodeposition technique.The electrochemical performance of the NMMSe electrodes was systematically investigated as a positive electrode.The NMMSe electrode prepared with a deposition time of 200 s(denoted as NMMSe-200)revealed a high areal/specific capacity of 439.4μAh cm^(−2)/225.6 mA h g^(−1) at 4 mA cm^(–2),along with excellent cycling stability.To further investigate the effect of deposition time on the nanostructure evaluation and electrochemical behavior,additional NMMSe electrodes were synthesized at the growth times of 100 and 300 s.For the negative electrode,activated carbon derived from pistachio shell waste(i.e.,porous activated carbon(PAC))was employed,demonstrating a high areal capacitance of 913.4 mF cm^(−2) and an excellent surface area of 320.6 m^(2)/g.Finally,a semi-solid-state hybrid capacitor(HC)cell was assembled using NMMSe-200 as the positive(+)electrode and PAC as the negative(-)electrode.The resulting NMMSe//PAC/nickel foam HC cell delivered an impressive areal capacitance of 928.8 mF cm^(−2) at 2 mA cm^(–2),a high energy density of 338.5μWh cm^(–2)(56.4 Wh kg^(−1)),and exceptional cycling stability.These results highlight the strong potential of NMMSe-200 electrodes for high-performance,wearable energy storage systems.展开更多
Alkynyl selenides were prepared under very mild conditions by reacting terminal alkynes with respective diorganic diselenides in the presence of potassium t-butoxide. The advantages of this protocol include the use of...Alkynyl selenides were prepared under very mild conditions by reacting terminal alkynes with respective diorganic diselenides in the presence of potassium t-butoxide. The advantages of this protocol include the use of readily available substrates and reagent and good yield of the products.展开更多
1,4-Dienyl selenides can be stereoselectively synthesized in one pot under mild conditions in good yields by the palladiumcatalyzed hydrostannylation of acetylenic selenides, followed by Stille coupling with allylic b...1,4-Dienyl selenides can be stereoselectively synthesized in one pot under mild conditions in good yields by the palladiumcatalyzed hydrostannylation of acetylenic selenides, followed by Stille coupling with allylic bromides.展开更多
Reduction of diaryldiselenides by the system of Cp2TiCl2/Bu'MgBr/THF gave the nucleophilic arylselenium complex. They reacted with diaryl iodonium salts to afford unsymmetrical diaryl selenides in high yields.
A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethyls...A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethylsilyl chloride under mild conditions. Presumably, the diselenides are cleaved by Sm/TMSCI system to form selemde anions, which then undergo SN2＇ substitution of Baylis-Hillman adducts to produce the （Z）-allyl selenides.展开更多
Two-dimensional Ti_(3)C_(2)T_(x) exhibits outstanding rate property and cycle performance in lithium-ion capacitors(LICs)due to its unique layered structure,excellent electronic conductivity,and high specific surface ...Two-dimensional Ti_(3)C_(2)T_(x) exhibits outstanding rate property and cycle performance in lithium-ion capacitors(LICs)due to its unique layered structure,excellent electronic conductivity,and high specific surface area.However,like graphene,Ti_(3)C_(2)T_(x) restacks during electrochemical cycling due to hydrogen bonding or van der Waals forces,leading to a decrease in the specific surface area and an increase in the diffusion distance of electrolyte ions between the interlayer of the material.Here,a transition metal selenide MoSe_(2) with a special three-stacked atomic layered structure,derived from metal-organic framework(MOF),is introduced into the Ti_(3)C_(2)T_(x) structure through a solvo-thermal method.The synergic effects of rapid Li+diffusion and pillaring effect from the MoSe_(2) and excellent conductivity from the Ti_(3)C_(2)T_(x) sheets endow the material with excellent electrochemical reaction kinetics and capacity.The composite Ti_(3)C_(2)T_(x)@MoSe_(2) material exhibits a high capacity over 300 mAh·g^(-1) at 150 mA·g^(-1) and excellent rate property with a specific capacity of 150 mAh·g^(-1) at 1500 mA·g^(-1).Addition-ally,the material shows a superior capacitive contribution of 86.0%at 2.0 mV·s^(-1) due to the fast electrochemical reactions.A Ti_(3)C_(2)T_(x)@MoSe_(2)//AC LIC device is also fabricated and exhibits stable cycle performance.展开更多
Two-dimensional(2D)MXenes are promising as electrode materials for energy storage,owing to their high electronic conductivity and low diffusion barrier.Unfortunately,similar to most 2D materials,MXene nanosheets easil...Two-dimensional(2D)MXenes are promising as electrode materials for energy storage,owing to their high electronic conductivity and low diffusion barrier.Unfortunately,similar to most 2D materials,MXene nanosheets easily restack during the electrode preparation,which degrades the electrochemical performance of MXene-based materials.A novel synthetic strategy is proposed for converting MXene into restacking-inhibited three-dimensional(3D)balls coated with iron selenides and carbon.This strategy involves the preparation of Fe_(2)O_(3)@carbon/MXene microspheres via a facile ultrasonic spray pyrolysis and subsequent selenization process.Such 3D structuring effectively prevents interlayer restacking,increases the surface area,and accelerates ion transport,while maintaining the attractive properties of MXene.Furthermore,combining iron selenides and carbon with 3D MXene balls offers many more sites for ion storage and enhances the structural robustness of the composite balls.The resultant 3D structured microspheres exhibit a high reversible capacity of 410 mAh g^(−1) after 200 cycles at 0.1 A g^(−1) in potassium-ion batteries,corresponding to the capacity retention of 97% as calculated based on 100 cycles.Even at a high current density of 5.0 A g^(−1),the composite exhibits a discharge capacity of 169 mAh g^(−1).展开更多
As a fundamental surface property of two-dimensional(2 D)materials,surface potential is critical for their emerging electronic applications and essential for van der Waals heterostructure engineering.Here,we report th...As a fundamental surface property of two-dimensional(2 D)materials,surface potential is critical for their emerging electronic applications and essential for van der Waals heterostructure engineering.Here,we report the surface potential of few-layer InSe.The effect of layer count,light intensity and different deposited substrates is considered.Few-layer InSe flakes were exfoliated from bulk InSe crystals on Si/SiO_(2)with 300-nm-thick thermal oxide and Si/SiO_(2)with 300-nm-thick thermal oxide and prefabricated micro-wells with 3μm in diameter.The samples were measured by Kelvin probe force microscopy and tuned by an integrated 405-nm(3.06 eV)laser.Based on the work function of SiO_(2)(5.00 eV),the work functions of supported and suspended InSe are determined.These results show that the work function of InSe decreases with the increase in the layer count of both supported InSe and suspended InSe.Besides,by introducing a tunable laser light,the influence of light intensity on surface potential of supported InSe was studied.The surface potential(SP)and surface potential shift between light and dark states(ASP=SP_(lignt)-SP_(dark))of supported InSe were measured and determined.These results present that the surface potential of supported InSe decreases with the increase in the light intensity and also decreases with the increase in the layer count.This is evident that light excites electrons,resulting in decreased surface potential,and the amount of electrons excited is correlated with light intensity.Meanwhile,⊿SP between light and dark states decreases with the increase in the layer count,which suggests that the influence of light illumination decreases with the increase in the layer count of few-layer InSe flakes.展开更多
Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaero...Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaerophobic three dimensional(3D)heterostructured nanowrinkles of bimetallic selenides consisting of crystalline NiSe2 and NiFe2Se4 grown on NiFe alloy(NiSe2/NiFe2Se4@NiFe)prepared by a thermal selenization procedure.In this unique 3D heterostructure,numerous nanowrinkles of NiSe2/NiFe2Se4 hybrid with a thickness of ~100 nm are grown on NiFe alloy in a uniform manner.Profiting by the large active surface area and high electronic conductivity,the superaerophobic NiSe2/NiFe2Se4@NiFe heterostructure exhibits excellent electrocatalytic activity and durability towards OER in alkaline media,outputting the low potentials of 1.53 and 1.54 V to achieve ultra-high current densities of 500 and 1000 mA cm^−2,respectively,which is among the most active Ni/Fe-based selenides,and even superior to the benchmark Ir/C catalyst.The in-situ derived FeOOH and NiOOH species from NiSe2/NiFe2Se4@NiFe are deemed to be efficient active sites for OER.展开更多
Cobalt selenide(CoSe_(2))has become a promising anode material for sodium-ion batteries(SIBs)due to its stable chemical properties,environmental friendliness,and high theoretical capacity.However,the undesirable rate ...Cobalt selenide(CoSe_(2))has become a promising anode material for sodium-ion batteries(SIBs)due to its stable chemical properties,environmental friendliness,and high theoretical capacity.However,the undesirable rate capacity and cycle stability of the anode materials largely limit its applications for SIBs due to the relatively low electronic conductivity and huge volume change during the Na+insertion/extraction.In this study,electrostatic spinning combined with a wet chemical method is employed to synthesize coral-like composite material(CNF@c-CoSe_(2)/C),which is composed of CoSe_(2)/carbon nanosheet arrays(CoSe_(2)/C)and carbon nanofibers(CNFs).CoSe_(2)/C nanoflakes derived from metal-organic frameworks(MOFs)with high surface area and the porous structure can inhibit the pulverization and amorphization of CoSe_(2) during charge and discharge processes,thus significantly keeping the stability of the microstructure.CNF can limit the overgrowth of nanosheets and serve as a conductive skeleton.Compared to two-dimensional CoSe_(2)/C nanoflakes and pure CoSe_(2) nanoparticles,the composite can expose more active sites and effectively accelerate the diffusion of Na+,which displays enhanced rate capability(266.5 mAh·g^(-1) at 5.0 A·g^(-1))and cycling stability(268.3 mAh·g^(-1) after 100 cycles at 1.0 A·g^(-1)).Moreover,the rational preparation strategy for metal selenide-based heterostructure material presents a new way for high-performance SIB s.展开更多
Demand of highly efficient earth-abundant transition metal-based electrocatalysts to replace noble metal materials for boosting oxygen evolution reaction(OER)is rapidly growing.Herein,an electrochemically exfoliated g...Demand of highly efficient earth-abundant transition metal-based electrocatalysts to replace noble metal materials for boosting oxygen evolution reaction(OER)is rapidly growing.Herein,an electrochemically exfoliated graphite(EG)foil supported bimetallic selenide encased in N-doped carbon(EG/(Co,Ni)Se2-NC)hybrid is developed and synthesized by a vapor-phase hydrothermal strategy and subsequent selenization process.The as-prepared EG/(Co,Ni)Se2-NC hybrid exhibits a core-shell structure where the particle diameter of(Co,Ni)Se2 core is about 70 nm and the thickness of N-doped carbon shell is approximately 5 nm.Benefitting from the synergistic effects between the combination of highly active Co species and improved electron transfer from Ni species,and N-doped carbon,the EG/(Co,Ni)Se2-NC hybrid shows remarkable electrocatalytic activity toward OER with a comparatively low overpotential of 258 mV at an current density of 10 mA cm?2 and a small Tafel slope of 73.3 mV dec?1.The excellent OER catalysis performance of EG/(Co,Ni)Se2-NC hybrid is much better than that of commercial Ir/C(343 mV at 10 mA cm?2 and 98.1 mV dec?1),and even almost the best among all previously reported binary CoNi selenide-based OER electrocatalysts.Furthermore,in situ electrochemical Raman spectroscopy combined with ex situ X-ray photoelectron spectroscopy analysis indicates that the superb OER catalysis activity can be attributed to the highly active Co-OOH species and modified electron transfer process from Ni element.展开更多
基金funding support from the National Key Research and Development Program of China(Grant No.2020YFB0408002)the Beijing Natural Science Foundation(Z240024)+2 种基金the National Natural Science Foundation of China(Grant Nos.22279083,22461160281,W2412076)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022B1515120006)the Central Guiding Local Science and Technology Development Special Fund Project(Grant No.ZYYD2024JD24)。
文摘Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing(No.06500227)the Fundamental Research Funds for the Central Universities(No.FRF-TP-22-091A1)+1 种基金National Natural Science Foundation of China(No.52200121),Chinese Universities Scientific Fund(No.00007713)the Guide special project(No.40103322).
文摘With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.
基金supported by the National Natural Science Foundation of China(22201244,22374125,21971221 and 21773203)the Yangzhou University Interdisciplinary Research Foundation for Chemistry Discipline of Targeted Support(yzuxk202010)+2 种基金High-Level Entrepreneurial and Innovative Talents Program of Jiangsu‘Qing Lan Project’in Colleges and Universities of Jiangsu ProvinceLvyangjinfeng Talent Program of Yangzhou,China Postdoctoral Science Foundation(2022M722688)。
文摘The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxometalate(POM)nanoclusters with high catalytic activity and cobalt selenide with strong polarity are initially complemented to construct a PMo_(12)/CoSe_(2)@NC/CNTs multifunctional separator that can simultaneously solve the above problems.A series of experimental and theoretical results demonstrate that the Keggin-type POM,H_(3)PMo_(12)O_(40)nH_(2)O(PMo_(12))nanoclusters could function as catalytic centers for sulfur-involved transformations,with the CoSe_(2)nanoparticles serving as adsorption sites for soluble polysulfides.Accordingly,the assembled battery with the PMo_(12)/CoSe_(2)@NC/CNTs modified separator achieves an initial discharge capacity of 1263.79 mA h g^(-1),maintaining 635.77 mA h g^(-1),with a capacity decay rate of 0.06%per cycle after 500 cycles at 3C.This work provides a strategic approach for incorporating POM nanoclusters with polar periodic nanomaterials in LSB separators,contributing to the development of multifunctional separator materials,thus promoting the advancement of energy storage systems.
基金supported by the Science and Technology Innovation Council of Shenzhen(No.KQTD20170810105439418)the National Key R&D Project from Minister of Science and Technology,China(No.2021YFB3200304)+2 种基金National Natural Science Foundation of China(Nos.6237129,52125205,U20A20166,61805015 and 61804011)the Natural Science Foundation of Beijing Municipality(No.Z180011)the Fundamental Research Funds for the Central Universities.
文摘Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic devices.However,the performance of TMDs-based devices is hampered by the suboptimal quality of metal electrodes contacting the atomically thin TMDs layers.Understanding the mechanisms that influence contact quality is crucial for advancing TMDs devices.In this study,we investigated the conductive properties of tungsten selenide(WSe_(2))-based devices with different film thicknesses.Using the transmission line method,a negative correlation between contact resistance and film thickness in multi-electrode devices was revealed.Additionally,repeatability tests conducted at varied temperatures indicated enhanced device stability with increasing film thickness.Theoretical analysis,supported by thermionic emission theory and thermal simulations,suggests that the degradation in electrical properties is primarily due to the thermal effect at the contact interface.Furthermore,we found that van der Waals contacts could mitigate the thermal effect through a metal transfer method.Our findings elucidate the critical role of contact resistance in the electronic performance of 2D material-based field-effect transistors(FETs),which further expands their potential in the next generation of electronic and optoelectronic devices.
基金supported by the National Natural Science Foundation of China(Nos.52130101 and 52271217)the Project of Science and Technology Development Plan of Jilin Province in China(Nos.20210402058GH,20220201114GX).
文摘Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some difficulties in exploring practical applications in which cycling stability and cycle life are awful owing to the shuttling effect of lithium polysulfides(LiPSs)and low sulfur utilization.In this work,by synthesizing Co_(3)Se_(4) nanoparticles onto N-doped carbon(NC)polyhedra interconnected with carbon nanotubes(CNTs),NC@Co_(3)Se_(4)/CNTs is proposed as a multifunctional sulfur carrier.The Co_(3)Se_(4) nanoparticles fleetly catalyze the conversion of LiPSs and availably immobilize LiPSs.Meanwhile,the NC polyhedral skeleton enhances the electronic conductivity of active sulfur,while the CNTs facilitate Li+diffusion and supply a mass of conductive channels.Density-functional theory(DFT)calculations demonstrate the relevant mechanisms.That is to say,the NC@Co_(3)Se_(4)/CNTs benefit from the synergistic effect of Co_(3)Se_(4) nanoparticles(highly catalytic ability and strong adsorbability for LiPSs)and the special carbonaceous structure,rapidly converting LiPSs and inhibiting the shuttle of LiPSs.Therefore,lithium-sulfur battery assembled with S/NC@Co_(3)Se_(4)/CNTs cathode as well as nitrogen and sulfur co-doped carbon-coated polypropylene(N,S-C/PP)separator possesses a high initial discharge capacity of 1413 mAh·g-1 at 0.12C and persistently circulates for 1000 cycles at 1C with a capacity attenuation rate per cycle of 0.034%.This work provides a realistic idea for the use of transition metal selenide in the field of high-performance LSBs.
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing (No.06500227)the Fundamental Research Funds for the Central Universities (No.FRF-TP-22-091A1).
文摘Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.
基金supported by the grants from the National Natural Science Foundation of China(No.22202098)the Natural Science Foundation of Henan Province(No.242300420199)。
文摘Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2018R1A6A1A03025708).
文摘Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a trimetallic nickel–magnesium-manganese selenide(NMMSe)electrode with a well-defined nanosphere morphology was prepared using a low-cost and rapid electrodeposition technique.The electrochemical performance of the NMMSe electrodes was systematically investigated as a positive electrode.The NMMSe electrode prepared with a deposition time of 200 s(denoted as NMMSe-200)revealed a high areal/specific capacity of 439.4μAh cm^(−2)/225.6 mA h g^(−1) at 4 mA cm^(–2),along with excellent cycling stability.To further investigate the effect of deposition time on the nanostructure evaluation and electrochemical behavior,additional NMMSe electrodes were synthesized at the growth times of 100 and 300 s.For the negative electrode,activated carbon derived from pistachio shell waste(i.e.,porous activated carbon(PAC))was employed,demonstrating a high areal capacitance of 913.4 mF cm^(−2) and an excellent surface area of 320.6 m^(2)/g.Finally,a semi-solid-state hybrid capacitor(HC)cell was assembled using NMMSe-200 as the positive(+)electrode and PAC as the negative(-)electrode.The resulting NMMSe//PAC/nickel foam HC cell delivered an impressive areal capacitance of 928.8 mF cm^(−2) at 2 mA cm^(–2),a high energy density of 338.5μWh cm^(–2)(56.4 Wh kg^(−1)),and exceptional cycling stability.These results highlight the strong potential of NMMSe-200 electrodes for high-performance,wearable energy storage systems.
基金the K.N.Toosi University of Technology Research Council for financial assistance
文摘Alkynyl selenides were prepared under very mild conditions by reacting terminal alkynes with respective diorganic diselenides in the presence of potassium t-butoxide. The advantages of this protocol include the use of readily available substrates and reagent and good yield of the products.
基金the National Natural Science Foundation of China (No.20462002)Natural Science Foundation of Jiangxi Province (No.2007GZW0172) for financial support.
文摘1,4-Dienyl selenides can be stereoselectively synthesized in one pot under mild conditions in good yields by the palladiumcatalyzed hydrostannylation of acetylenic selenides, followed by Stille coupling with allylic bromides.
文摘Reduction of diaryldiselenides by the system of Cp2TiCl2/Bu'MgBr/THF gave the nucleophilic arylselenium complex. They reacted with diaryl iodonium salts to afford unsymmetrical diaryl selenides in high yields.
基金Project (No. 2004C21032) supported by the Key Technologies R &D Program of Zhejiang Province, China
文摘A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethylsilyl chloride under mild conditions. Presumably, the diselenides are cleaved by Sm/TMSCI system to form selemde anions, which then undergo SN2＇ substitution of Baylis-Hillman adducts to produce the （Z）-allyl selenides.
基金supported by the National Natural Science Foundation of China(No.51972023)。
文摘Two-dimensional Ti_(3)C_(2)T_(x) exhibits outstanding rate property and cycle performance in lithium-ion capacitors(LICs)due to its unique layered structure,excellent electronic conductivity,and high specific surface area.However,like graphene,Ti_(3)C_(2)T_(x) restacks during electrochemical cycling due to hydrogen bonding or van der Waals forces,leading to a decrease in the specific surface area and an increase in the diffusion distance of electrolyte ions between the interlayer of the material.Here,a transition metal selenide MoSe_(2) with a special three-stacked atomic layered structure,derived from metal-organic framework(MOF),is introduced into the Ti_(3)C_(2)T_(x) structure through a solvo-thermal method.The synergic effects of rapid Li+diffusion and pillaring effect from the MoSe_(2) and excellent conductivity from the Ti_(3)C_(2)T_(x) sheets endow the material with excellent electrochemical reaction kinetics and capacity.The composite Ti_(3)C_(2)T_(x)@MoSe_(2) material exhibits a high capacity over 300 mAh·g^(-1) at 150 mA·g^(-1) and excellent rate property with a specific capacity of 150 mAh·g^(-1) at 1500 mA·g^(-1).Addition-ally,the material shows a superior capacitive contribution of 86.0%at 2.0 mV·s^(-1) due to the fast electrochemical reactions.A Ti_(3)C_(2)T_(x)@MoSe_(2)//AC LIC device is also fabricated and exhibits stable cycle performance.
基金supported by the National Research Foundation of Korea(NRF)grant funded by Korea government(NRF-2019R1A2C2088047 and NRF-2020R1C1C1003375).
文摘Two-dimensional(2D)MXenes are promising as electrode materials for energy storage,owing to their high electronic conductivity and low diffusion barrier.Unfortunately,similar to most 2D materials,MXene nanosheets easily restack during the electrode preparation,which degrades the electrochemical performance of MXene-based materials.A novel synthetic strategy is proposed for converting MXene into restacking-inhibited three-dimensional(3D)balls coated with iron selenides and carbon.This strategy involves the preparation of Fe_(2)O_(3)@carbon/MXene microspheres via a facile ultrasonic spray pyrolysis and subsequent selenization process.Such 3D structuring effectively prevents interlayer restacking,increases the surface area,and accelerates ion transport,while maintaining the attractive properties of MXene.Furthermore,combining iron selenides and carbon with 3D MXene balls offers many more sites for ion storage and enhances the structural robustness of the composite balls.The resultant 3D structured microspheres exhibit a high reversible capacity of 410 mAh g^(−1) after 200 cycles at 0.1 A g^(−1) in potassium-ion batteries,corresponding to the capacity retention of 97% as calculated based on 100 cycles.Even at a high current density of 5.0 A g^(−1),the composite exhibits a discharge capacity of 169 mAh g^(−1).
基金the Key-Area Research and Development Program of Guangdong Province(No.2018B010109009)the Shenzhen Science and Technology Innovation Committee(Nos.JCYJ20170818155752559 and JCYJ20170818160815002)+3 种基金the Instrument Developing Project of Chinese Academy of Sciences(No.ZDKYYQ20180004)the National Natural Science Foundation of China(No.11872203)the National Natural Science Foundation of China for Creative Research Groups(No.51921003)support of the China Scholarship Council。
文摘As a fundamental surface property of two-dimensional(2 D)materials,surface potential is critical for their emerging electronic applications and essential for van der Waals heterostructure engineering.Here,we report the surface potential of few-layer InSe.The effect of layer count,light intensity and different deposited substrates is considered.Few-layer InSe flakes were exfoliated from bulk InSe crystals on Si/SiO_(2)with 300-nm-thick thermal oxide and Si/SiO_(2)with 300-nm-thick thermal oxide and prefabricated micro-wells with 3μm in diameter.The samples were measured by Kelvin probe force microscopy and tuned by an integrated 405-nm(3.06 eV)laser.Based on the work function of SiO_(2)(5.00 eV),the work functions of supported and suspended InSe are determined.These results show that the work function of InSe decreases with the increase in the layer count of both supported InSe and suspended InSe.Besides,by introducing a tunable laser light,the influence of light intensity on surface potential of supported InSe was studied.The surface potential(SP)and surface potential shift between light and dark states(ASP=SP_(lignt)-SP_(dark))of supported InSe were measured and determined.These results present that the surface potential of supported InSe decreases with the increase in the light intensity and also decreases with the increase in the layer count.This is evident that light excites electrons,resulting in decreased surface potential,and the amount of electrons excited is correlated with light intensity.Meanwhile,⊿SP between light and dark states decreases with the increase in the layer count,which suggests that the influence of light illumination decreases with the increase in the layer count of few-layer InSe flakes.
基金financially supported by the National Natural Science Foundation of China(21922811,51702284,and 21878270)Zhejiang Provincial Natural Science Foundation of China(LR19B060002)the Startup Foundation for Hundred-Talent Program of Zhejiang University.
文摘Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaerophobic three dimensional(3D)heterostructured nanowrinkles of bimetallic selenides consisting of crystalline NiSe2 and NiFe2Se4 grown on NiFe alloy(NiSe2/NiFe2Se4@NiFe)prepared by a thermal selenization procedure.In this unique 3D heterostructure,numerous nanowrinkles of NiSe2/NiFe2Se4 hybrid with a thickness of ~100 nm are grown on NiFe alloy in a uniform manner.Profiting by the large active surface area and high electronic conductivity,the superaerophobic NiSe2/NiFe2Se4@NiFe heterostructure exhibits excellent electrocatalytic activity and durability towards OER in alkaline media,outputting the low potentials of 1.53 and 1.54 V to achieve ultra-high current densities of 500 and 1000 mA cm^−2,respectively,which is among the most active Ni/Fe-based selenides,and even superior to the benchmark Ir/C catalyst.The in-situ derived FeOOH and NiOOH species from NiSe2/NiFe2Se4@NiFe are deemed to be efficient active sites for OER.
基金financially supported by the National Natural Science Foundation of China(Nos.51603092 and 21706103)the Natural Science Foundation of Jiangsu Province(Nos.BK20160537 and BK20170549)China Postdoctoral Science Foundation(No.2019T120393)。
文摘Cobalt selenide(CoSe_(2))has become a promising anode material for sodium-ion batteries(SIBs)due to its stable chemical properties,environmental friendliness,and high theoretical capacity.However,the undesirable rate capacity and cycle stability of the anode materials largely limit its applications for SIBs due to the relatively low electronic conductivity and huge volume change during the Na+insertion/extraction.In this study,electrostatic spinning combined with a wet chemical method is employed to synthesize coral-like composite material(CNF@c-CoSe_(2)/C),which is composed of CoSe_(2)/carbon nanosheet arrays(CoSe_(2)/C)and carbon nanofibers(CNFs).CoSe_(2)/C nanoflakes derived from metal-organic frameworks(MOFs)with high surface area and the porous structure can inhibit the pulverization and amorphization of CoSe_(2) during charge and discharge processes,thus significantly keeping the stability of the microstructure.CNF can limit the overgrowth of nanosheets and serve as a conductive skeleton.Compared to two-dimensional CoSe_(2)/C nanoflakes and pure CoSe_(2) nanoparticles,the composite can expose more active sites and effectively accelerate the diffusion of Na+,which displays enhanced rate capability(266.5 mAh·g^(-1) at 5.0 A·g^(-1))and cycling stability(268.3 mAh·g^(-1) after 100 cycles at 1.0 A·g^(-1)).Moreover,the rational preparation strategy for metal selenide-based heterostructure material presents a new way for high-performance SIB s.
基金Y.Hou expresses appreciation of the assistance of the NSFC 51702284 and 21878270Zhejiang Provincial Natural Science Foundation of China(LR19B060002)the Startup Foundation for Hundred-Talent Program of Zhejiang University(112100-193820101/001/022).
文摘Demand of highly efficient earth-abundant transition metal-based electrocatalysts to replace noble metal materials for boosting oxygen evolution reaction(OER)is rapidly growing.Herein,an electrochemically exfoliated graphite(EG)foil supported bimetallic selenide encased in N-doped carbon(EG/(Co,Ni)Se2-NC)hybrid is developed and synthesized by a vapor-phase hydrothermal strategy and subsequent selenization process.The as-prepared EG/(Co,Ni)Se2-NC hybrid exhibits a core-shell structure where the particle diameter of(Co,Ni)Se2 core is about 70 nm and the thickness of N-doped carbon shell is approximately 5 nm.Benefitting from the synergistic effects between the combination of highly active Co species and improved electron transfer from Ni species,and N-doped carbon,the EG/(Co,Ni)Se2-NC hybrid shows remarkable electrocatalytic activity toward OER with a comparatively low overpotential of 258 mV at an current density of 10 mA cm?2 and a small Tafel slope of 73.3 mV dec?1.The excellent OER catalysis performance of EG/(Co,Ni)Se2-NC hybrid is much better than that of commercial Ir/C(343 mV at 10 mA cm?2 and 98.1 mV dec?1),and even almost the best among all previously reported binary CoNi selenide-based OER electrocatalysts.Furthermore,in situ electrochemical Raman spectroscopy combined with ex situ X-ray photoelectron spectroscopy analysis indicates that the superb OER catalysis activity can be attributed to the highly active Co-OOH species and modified electron transfer process from Ni element.
