Dielectric elastomer actuators (DEAs) artificial muscle is a typical interdisciplinary research category, which has developed by leaps and bounds in the past 20 years, showing great application prospects in various fi...Dielectric elastomer actuators (DEAs) artificial muscle is a typical interdisciplinary research category, which has developed by leaps and bounds in the past 20 years, showing great application prospects in various fields. Upon external electrical stimulation, dielectric elastomers (DEs) display large deformation, high energy density and fast response, affording a promising material candidate for soft robotics. Herein, the working mechanisms, commonly used materials as well as the concepts for improving the performance of DEA materials are introduced. Various DEA driven soft robots, including soft grippers, bioinspired artificial arms, crawling/walking/underwater/flying/jumping soft robots and tunable lenses, are then described in detail. Finally, the main challenges of DEA driven soft robots are summarized, and some perspectives for promoting the practical application of DEAs are also proposed.展开更多
The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing...The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing CO_(2) to C_(2+)products,the instability of Cu^(+)species,which tend to reduce to Cu~0 at cathodic potentials during CO_(2) reduction,poses a significant challenge.Here,we report the development of SmCu_(2)O and investigate the influence of f-d orbital hybridization on the CO_(2) reduction reaction (CO_(2)RR).Supported by density functional theory (DFT) calculations,our experimental results demonstrate that hybridization between Sm^(3+)4f and Cu^(+)3d orbitals not only improves the adsorption of *CO intermediates and increases CO coverage to stabilize Cu^(+) but also facilitates CO_(2) activation and lowers the energy barriers for CAC coupling.Notably,Sm-Cu_(2)O achieves a Faradaic efficiency for C_(2)H_(4) that is 38%higher than that of undoped Cu_(2)O.Additionally,it sustains its catalytic activity over an extended operational period exceeding 7 h,compared to merely 2 h for the undoped sample.This research highlights the potential of fd orbital hybridization in enhancing the efficacy of copper-based catalysts for CO_(2)RR,pointing towards a promising direction for the development of durable,high-performance electrocatalysts for sustainable chemical synthesis.展开更多
Hydrogen peroxide(H_(2)O_(2))is a green oxidant that has been widely used.The direct synthesis of hydrogen peroxide(DSHP)offers significant advantages in terms of high atomic economy and environmentally friendly effec...Hydrogen peroxide(H_(2)O_(2))is a green oxidant that has been widely used.The direct synthesis of hydrogen peroxide(DSHP)offers significant advantages in terms of high atomic economy and environmentally friendly effects.However,due to the inevitable side reactions and severe mass transfer limitations,it is still challenging to balance the selectivity and activity for the DSHP.Combining theoretical understanding with the controllable synthesis of nanocatalysts may significantly facilitate the design of“dream catalysts”for the DSHP.In this work,the main factors affecting the reaction performance of catalysts and the active sites of catalysts have been reviewed and discussed in detail.The development and design of catalysts with high efficiency were introduced from three aspects:the catalyst support,active component and atomic impurity.In addition,the coupling of DSHP and other oxidation reactions to realize one-pot in situ oxidation reactions was comprehensively emphasized,which showed essential guiding significance for the future development of H_(2)O_(2).展开更多
Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their...Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their application as thermal interface materials.Herein,lamellarstructured polyamic acid salt/graphene oxide(PAAS/GO)hybrid aerogels are constructed by bidirectional freezing of PAAS/GO suspension followed by lyophilization.Subsequently,PAAS monomers are polymerized to polyimide(PI),while GO is converted to thermally reduced graphene oxide(RGO)during thermal annealing at 300℃.Final graphitization at 2800℃ converts PI to graphitized carbon with the inductive effect of RGO,and simultaneously,RGO is thermally reduced and healed to high-quality graphene.Consequently,lamellar-structured graphene aerogels with superior through-plane thermal conduction capacity are fabricated for the first time,and its superior through-plane thermal conduction capacity results from its vertically aligned and closely stacked high-quality graphene lamellae.After vacuum-assisted impregnation with epoxy,the resultant epoxy composite with 2.30 vol% of graphene exhibits an outstanding through-plane thermal conductivity of as high as 20.0 W m^−1 K^−1,100 times of that of epoxy,with a record-high specific thermal conductivity enhancement of 4310%.Furthermore,the lamellar-structured graphene aerogel endows epoxy with a high fracture toughness,~1.71 times of that of epoxy.展开更多
In the present study,we propose a novel electrode material ofβ-nickel hydroxide covering nickel/aluminum layered double hydroxides via a facile complexation–precipitation method.The as-obtained materials with 3-dime...In the present study,we propose a novel electrode material ofβ-nickel hydroxide covering nickel/aluminum layered double hydroxides via a facile complexation–precipitation method.The as-obtained materials with 3-dimensional nanostructures are further utilized as highly capable electrode material in nickel–metal hydride batteries.The electrochemical test results demonstrated theβ-nickel hydroxide covering nickel/aluminum-layered double hydroxides with 28%ofβ-nickel hydroxide provided a superior specific capacity value of 452 m A·h·g-1 in a current density of 5 A·g-1 using 6 M KOH as electrolyte as compared with other materials.In addition,the optimized sample displays an outstanding cyclic stability along with a huge specific capacity value of320 m Ah·g-1,and very small decay rate of 3.3%at 50 A·g-1 after 3000 cycles of charge/discharge test.These indicate that the newly designed material with nanostructures not only provides an efficient contact interface between electrolyte and active species and facilitates the transport of electrons and ions,but also protects the 3-dimensional nickel/aluminum layered double hydroxides,achieving a high specific capacity,fast redox reaction and excellent long-term cyclic stability.Therefore,theβ-nickel hydroxide covering nickel/aluminum layered double hydroxides with superior electrochemical performance is predictable to be a gifted electrode material in nickel–metal hydride batteries.展开更多
The highly integrated and miniaturized next-generation electronic products call for high-performance electromagnetic interference(EMI)shielding materials to assure the normal operation of their closely assembled compo...The highly integrated and miniaturized next-generation electronic products call for high-performance electromagnetic interference(EMI)shielding materials to assure the normal operation of their closely assembled components.However,the most current techniques are not adequate for the fabrication of shielding materials with programmable structure and controllable shielding efficiency.Herein,we demonstrate the direct ink writing of robust and highly conductive Ti3C2Tx MXene frames with customizable structures by using MXene/AlOOH inks for tunable EMI shielding and electromagnetic wave-induced thermochromism applications.The as-printed frames are reinforced by immersing in AlCl_(3)/HCl solution to remove the electrically insulating AlOOH nanoparticles,as well as cross-link the MXene sheets and fuse the filament interfaces with aluminum ions.After freeze-drying,the resultant robust and porous MXene frames exhibit tunable EMI shielding efficiencies in the range of 25-80 dB with the highest electrical conductivity of 5323 S m−1.Furthermore,an electromagnetic wave-induced thermochromic MXene pattern is assembled by coating and curing with thermochromic polydimethylsiloxane on a printed MXene pattern,and its color can be changed from blue to red under the high-intensity electromagnetic irradiation.This work demonstrates a direct ink printing of customizable EMI frames and patterns for tuning EMI shielding efficiency and visualizing electromagnetic waves.展开更多
Water pollution caused by highly toxic Cd(II), Pb(II), and Cr(VI) is a serious problem. In the present work,a green and low-cost adsorbent of g-C_3N_4 nanosheets was developed with superior capacity for both cationic ...Water pollution caused by highly toxic Cd(II), Pb(II), and Cr(VI) is a serious problem. In the present work,a green and low-cost adsorbent of g-C_3N_4 nanosheets was developed with superior capacity for both cationic and anionic heavy metals. The adsorbent was easily fabricated through one-step calcination of guanidine hydrochloride with thickness less than 1.6 nm and specific surface area of 111.2 m^2·g^(-1). Kinetic and isotherm studies suggest that the adsorption is an endothermic chemisorption process, occurring on the energetically heterogeneous surface based on a hybrid mechanism of multilayer and monolayer adsorption. The tri-s-triazine units and surface N-containing groups of g-C_3N_4 nanosheets are proposed to be responsible for the adsorption process.Further study on pH demonstrates that electrostatic interaction plays an important role. The maximum adsorption capacity of Cd(II), Pb(II), and Cr(VI) on g-C_3N_4 nanosheets is 123.205 mg·g^(-1), 136.571 mg·g^(-1),and 684.451 mg·g^(-1), respectively. The better adsorption performance of the adsorbent than that of the recently reported nanomaterials and low-cost adsorbents proves its great application potential in the removal of heavy metal contaminants from wastewater. The present paper developed a promising adsorbent which will certainly find applications in wastewater treatment and also provides guiding significance in designing adsorption processes.展开更多
Lithium-sulfur(Li-S) battery is one of the best candidates for the next-generation energy storage system due to its high theoretical capacity(1675 mA h-1),low cost and environment friendliness.However,lithium(Li) dend...Lithium-sulfur(Li-S) battery is one of the best candidates for the next-generation energy storage system due to its high theoretical capacity(1675 mA h-1),low cost and environment friendliness.However,lithium(Li) dendrites formation and polysulfide shuttle effect are two major challenges that limit the commercialization of Li-S batteries.Here we design a facile bifunctional interlayer of gelatin-based fibers(GFs),aiming to protect the Li anode surface from the dendrites growth and also hinder the polysulfide shuttle effect.We reveal that the 3D structural network of GFs layer with abundant polar sites helps to homogenize Li-ion flux,leading to uniform Li-ion deposition.Meanwhile,the polar moieties also immobilize the lithium polysulfides and protect the Li metal from the side-reaction.As a result,the anodeprotected batteries have shown significantly enhanced performance.A high coulombic efficiency of 96% after 160 cycles has been achieved in the Li-Cu half cells.The Li-Li symmetric cells exhibit a prolonged lifespan for 800 h with voltage hysteresis(10 mV).With the as-prepared GFs layer,the Li-S battery shows approximately 14% higher capacity retention than the pristine battery at 0.5 C after 100 cycles.Our work presents that this gelatin-based bi-functional interlayer provides a viable strategy for the manufacturing of advanced Li-S batteries.展开更多
Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al me...Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al metal oxides(represented as Zn2ZrxAl-MMO)in light of the structural topotactic transformation of Zn2ZrxAl-hydrotalcite precursors(Zn2ZrxAl-LDH).The resulting Zn2ZrxAl-MMO catalysts were employed in the conversion of ethanol to diethyl carbonate.The Zr^4+ ion content of the LDH precursor plays a key role in modulating the acid-base properties and determining catalytic performance:the Zn2Zr0.1Al-MMO sample exhibits the optimal catalytic behavior with a diethyl carbonate(DEC)yield of 42.1%,which is the highest reported for metal oxide catalysts.Structure-property correlation investigations revealed that the synergic catalysis between medium-strong basic sites and weak acid sites plays a predominant role in the catalytic behavior.Furthermore,in situ Fourier transform infrared measurements showed that the weak acidic site promotes activation adsorption of the reactant(urea)and the intermediate product(ethyl carbamate),while the medium-strong basic site accelerates ethanol activation.Moreover,the Zn2Zr0.1Al-MMO catalyst has the advantages of cost effectiveness,good stability,and reusability.Therefore,the acid-base bifunctional catalysts developed in this work can be employed as promising candidates in acid-base catalytic reactions such as ethanol conversion.展开更多
The synthesis of fluorescent nanomaterials has received considerable attention due to the great potential of these materials for a wide range of applications, from chemical sensing through bioimaging to optoelectron- ...The synthesis of fluorescent nanomaterials has received considerable attention due to the great potential of these materials for a wide range of applications, from chemical sensing through bioimaging to optoelectron- ics. Herein, we report a facile and scalable approach to prepare fluorescent carbon dots (FCDs) via a one-pot reaction of citric acid with ethylenediamine at 150 ℃ under ambient air pressure. The resultant FCDs pos- sess an optical bandgap of 3.4 eV and exhibit strong excitation-wavelength-independent blue emission (λEm = 450 nm) under either one- or two-photon excitation. Owing to their low cytotoxicity and long fluorescence lifetime, these FCDs were successfully used as internalized fluorescent probes in human cancer cell lines (HeLa cells) for two-photon excited imaging of cells by fluorescence lifetime imaging microscopy with a high-contrast resolution. They were also homogenously mixed with commercial inks and used to draw fluo- rescent patterns on normal papers and on many other substrates (e.g., certain flexible plastic films, textiles, and clothes). Thus, these nanomaterials are promising for use in solid-state fluorescent sensing, security labeling, and wearable optoelectronics.展开更多
C1 chemistry is the essence of coal chemistry and natural gas chemistry. Catalytic methods to efficiently convert C1 molecules into fuels and chemicals have been extensively studied. Syngas(CO +H_2) conversion is t...C1 chemistry is the essence of coal chemistry and natural gas chemistry. Catalytic methods to efficiently convert C1 molecules into fuels and chemicals have been extensively studied. Syngas(CO +H_2) conversion is the most important industrial reaction system in C1 chemistry, and Fe and Co catalysts, two major industrial catalysts, have been the focus of fundamental research and industrial application. In the last decade, considerable research efforts have been devoted to discoveries concerning catalyst structure and increasing market demands for olefins and oxygenates. Since the development of efficient catalysts would strongly benefit from catalyst design and the establishment of a new reaction system, this review comprehensively overviews syngas conversion in three main reactions, highlights the advances recently made and the challenges that remain open, and will stimulate future research activities. The first part of the review summarizes the breakthroughs in Fischer-Tropsch synthesis regarding the optimization of activity and stability, determination of the active phase, and mechanistic studies. The second part overviews the modulation of catalytic structure and product selectivity for Fischer-Tropsch to olefins(FTO). Catalysts designed to produce higher alcohols, as well as to tune product selectivity in C1 chemistry, are described in the third section. Finally, present challenges in syngas conversion are proposed, and the solutions and prospects are discussed from the viewpoint of fundamental research and practical application. This review summarizes the latest advances in the design, preparation, and application of Fe/Co-based catalysts toward syngas conversion and presents the challenges and future directions in producing value-added fuels.展开更多
Cost effective separation of acetylene(C_2H_2)and ethylene(C_2H_4)is of key importance to obtain essential chemical raw materials for polymer industry.Due to the low compression limit of C_2H_2,there is an urgent dema...Cost effective separation of acetylene(C_2H_2)and ethylene(C_2H_4)is of key importance to obtain essential chemical raw materials for polymer industry.Due to the low compression limit of C_2H_2,there is an urgent demand to develop suitable materials for efficiently separating the two gases under ambient conditions.In this paper,we provided a high-throughput screening strategy to study porous metal-organic frameworks(MOFs)containing open metal sites(OMS)for C_2H_2/C_2H_4 separation,followed by a rational design of novel MOFs in-silico.A set of accurate force fields was established from ab initio calculations to describe the critical role of OMS towards guest molecules.From a large-scale computational screening of 916 experimental Cu-paddlewheel-based MOFs,three materials were identified with excellent separation performance.The structure-performance relationships revealed that the optimal materials should have the largest cavity diameter around 5-10?and pore volume in-between 0.3-1.0 cm^3 g^(-1).Based on the systematic screening study result,three novel MOFs were further designed with the incorporation of fluorine functional group.The results showed that Cu-OMS and the-F group on the aromatic rings close to Cu sites could generate a synergistic effect on the preferential adsorption of C_2H_2 over C_2H_4,leading to a remarkable improvement of C_2H_2 separation performance of the materials.The findings could provide insight for future experimental design and synthesis of high-performance nanostructured materials for C_2H_2/C_2H_4 separation.展开更多
It is of significance to design of stable and cost-effective electrocatalyst for water splitting with high efficiency in an alkaline medium.The major obstacles for practical application of water splitting devices are ...It is of significance to design of stable and cost-effective electrocatalyst for water splitting with high efficiency in an alkaline medium.The major obstacles for practical application of water splitting devices are lack of high-efficiency and low-cost electrocatalysts with low overpotential for both HER and OER.In this paper,we report a NiFe alloy decorated NiCoO2 hollow polyhedron(denoted as Ni Fe–Ni Co O2)by using[NiFe(CN)6]- intercalated NiCo–LDH as precursor.As evidenced by the electrochemical active surface area,the resultant Ni Fe–Ni Co O2 composite shows unique hollow nanostructure,which can not only provide abundant mass transport channels,but also increase the contact area of the NiFe–Ni Co O2 material with the electrolyte.The overpotential(η)demand is 286 mV for OER and 102 mV for HER at the current density of 10 mA/cm2 in an alkaline medium of 1 M KOH for the NiFe/NiCoO2 composite.This work provides a new pathway for preparation of the highly efficient bifunctional electrocatalysts for water splitting.展开更多
An electronic-nose is developed based on eight quartz-crystal-microbalance (QCM) gas sensors in a sensor box, and is used to detect Chinese liquors at room temperature. Each sensor is a highly-accurate and highly-sens...An electronic-nose is developed based on eight quartz-crystal-microbalance (QCM) gas sensors in a sensor box, and is used to detect Chinese liquors at room temperature. Each sensor is a highly-accurate and highly-sensitive oscillator that has experienced airflow disturbances under the condition of varying room temperatures due to unstable flow-induced forces on the sensors surfaces. The three-dimensional (3D) nature of the airflow inside the sensor box and the interactions of the airflow on the sensors surfaces at different temperatures are studied by computational fluid dynamics (CFD) tools. Higher simulation accuracy is achieved by optimizing meshes, meshing the computational domain using a fine unstructural tetrahedron mesh. An optimum temperature, 30 ℃, is obtained by analyzing the distributions of velocity streamlines and the static pressure, as well as the flow-induced forces over time, all of which may be used to improve the identification accuracy of the electronic-nose for achieving stable and repeatable signals by removing the influence of temperature.展开更多
The present paper reports a new fluoride-free and energy-saving lead electrolytic refining process in order to solve the serious problems of the existing Betts lead electrorefining process, such as low production effi...The present paper reports a new fluoride-free and energy-saving lead electrolytic refining process in order to solve the serious problems of the existing Betts lead electrorefining process, such as low production efficiency,high energy consumption and fluorine pollution. In the process, a mixed solution of perchloric acid and lead perchlorate(HClO4-Pb(ClO4)2) with the additives of gelatin and sodium lignin sulfonate is employed as the new electrolyte. The cathodic polarization curves show that HClO4 is very stable, and there is no any reduction reaction of HClO4 during the electrolytic process. The redox reactions of lead ions in HClO4 solution are very reversible with an ultrahigh capacity efficiency, so the HClO4 acts as a stable support electrolyte with higher ionic conductivity than the traditional H2SiF6 electrolyte. The results of the scale-up experiments show that under the optimal conditions of 2.8 mol·L-1 HClO4, 0.4 mol·L-1 Pb(ClO4)2 and electrolysis temperature of 45 ℃, the energy consumption is as low as 24.5 kW·h·(t Pb)-1 , only about 20% of that by Betts method at the same current density of 20 mA·cm-2, and the purity of the refined lead is up to 99.9992%, much higher than that specified by Chinese national standard(99.994%, GB/T 469-2013) and European standard(99.99%, EN 12659–1999).展开更多
Trace environmental pollutants have become a serious problem with special attention on the hazardous heavy metals, refractory organics, and pathogenic microorganisms. With coupling biosorption and photocatalysis to de...Trace environmental pollutants have become a serious problem with special attention on the hazardous heavy metals, refractory organics, and pathogenic microorganisms. With coupling biosorption and photocatalysis to develop biomaterial/TiO2 composite photocatalysts is a promising method to remove these trace pollutants because of the synergistic effect. Biomaterials provide multiple function groups which can selectively and efficiently enrich trace pollutants onto the surface of the photocatalysts, thus facilitating the following transformation mediated by TiO2 photocatalysis. Biomaterials can also help the dispersion and recovery of TiO2, or even modify the band structure of TiO2. The fabrication of chitosan/TiO2, cellulose/TiO2, as well as other biomaterial/TiO2 composite photocatalysts is discussed in detail in this review. The application significance of these composite photocatalysts for the selective removal of trace pollutants is also addressed. Several problems should be solved before the realistic applications can be achieved as discussed in the final section.展开更多
With advances in material science and a more in-depth understanding of device engineering,the power conversion efficiency(PCE)of solution-processed organic photovoltaic(OPV)cells have significantly boosted in the past...With advances in material science and a more in-depth understanding of device engineering,the power conversion efficiency(PCE)of solution-processed organic photovoltaic(OPV)cells have significantly boosted in the past few years.In 2019,a high PCE of 15.7%was achieved in the OPV cells adopting a wide bandgap polymer PM6 and a new emerging non-fullerene acceptor Y6.Such outstanding performance has attracted lots of research attention,driving considerable efforts to improve or take advantage of the high-performance PM6:Y6-based system.In this review,we first concentrate on the structural characteristics of PM6 and Y6 with the focus on understanding why their combination for OPV application can obtain such high efficiency.We also update the recent progress in highly efficient PM6:Y6-based OPV cells via various optimizing strategies.Then we summarize the other applications of the PM6:Y6-based system in semi-transparent,flexible or lay e-by-layer devices.The prospects for future OPV studies will be suggested in the end.展开更多
Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-s...Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction.Herein,atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery(termed as Fe-NSC) was synthesized,X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N3)(N-C-S).By enabling precisely localized S doping,the electronic structure of Fe-N4 moiety could be mediated,leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center.Density functional theory simulation suggested that more negative charge density would be localized over Fe-N4 moiety after S doping,allowing weakened binding capability to *OH intermediates and faster charge transfer from Fe center to O species.Electrochemical measurements revealed that the Fe-NSC sample exhibited significantly enhanced oxygen reduction reaction performance compared to the S-free Fe-NC material(termed as Fe-NC),showing an excellent onset potential of 1.09 V and half-wave potential of 0.92 V in 0.1 M KOH.Our work may enlighten relevant studies regarding to accessing improvement on the catalytic performance of atomically dispersed M-NC materials by managing precisely tuned local environments of M-Nx moiety.展开更多
A precise understanding of the redox chemistry of Nm-Mn+(like N4-Fe^(2+))systems is essential for fundamental studies and rational design of Nm-Mn+-based electrocatalysts for the oxygen reduction reaction(ORR).Herein,...A precise understanding of the redox chemistry of Nm-Mn+(like N4-Fe^(2+))systems is essential for fundamental studies and rational design of Nm-Mn+-based electrocatalysts for the oxygen reduction reaction(ORR).Herein,three different iron phthalocyanines(FePcs)adsorbed on carbon nanotubes((NH2)4FePc@CNTs,(t-Bu)4FePc@CNTs,and FePc@CNTs)were evaluated to demonstrate the effect of the electron donating power of the substituents on the Fe^(3+)/Fe^(2+)redox potential of FePc@CNTs and the role of these composites as ORR mediators in alkaline media.The Fe^(3+)/Fe^(2+)redox potential of the FePcs was found to shift towards the cathodic region upon substitution with electron-donating groups.This up-field shift in the eg-orbital leads to a lower overlap between the onset potential of the Fe^(3+)/Fe^(2+)redox couple and that of the ORR,and thus,the ORR activity decreased in the following order based on the substitution of FePc:-H>-t-Bu>-NH2.展开更多
Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through soluti...Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.展开更多
基金support from the National Natural Science Foundation of China(Grant No.51525301)the Talent Cultivation of State Key Laboratory of Organic-Inorganic Composites(No.OIC-D2021002).
文摘Dielectric elastomer actuators (DEAs) artificial muscle is a typical interdisciplinary research category, which has developed by leaps and bounds in the past 20 years, showing great application prospects in various fields. Upon external electrical stimulation, dielectric elastomers (DEs) display large deformation, high energy density and fast response, affording a promising material candidate for soft robotics. Herein, the working mechanisms, commonly used materials as well as the concepts for improving the performance of DEA materials are introduced. Various DEA driven soft robots, including soft grippers, bioinspired artificial arms, crawling/walking/underwater/flying/jumping soft robots and tunable lenses, are then described in detail. Finally, the main challenges of DEA driven soft robots are summarized, and some perspectives for promoting the practical application of DEAs are also proposed.
基金Financial support from the National Natural Science Foundation of China(grant nos.22379006,21575016,U20A20154,22279005)from the National Program for Support of Top-notch Young Professionals is gratefully acknowledged。
文摘The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing CO_(2) to C_(2+)products,the instability of Cu^(+)species,which tend to reduce to Cu~0 at cathodic potentials during CO_(2) reduction,poses a significant challenge.Here,we report the development of SmCu_(2)O and investigate the influence of f-d orbital hybridization on the CO_(2) reduction reaction (CO_(2)RR).Supported by density functional theory (DFT) calculations,our experimental results demonstrate that hybridization between Sm^(3+)4f and Cu^(+)3d orbitals not only improves the adsorption of *CO intermediates and increases CO coverage to stabilize Cu^(+) but also facilitates CO_(2) activation and lowers the energy barriers for CAC coupling.Notably,Sm-Cu_(2)O achieves a Faradaic efficiency for C_(2)H_(4) that is 38%higher than that of undoped Cu_(2)O.Additionally,it sustains its catalytic activity over an extended operational period exceeding 7 h,compared to merely 2 h for the undoped sample.This research highlights the potential of fd orbital hybridization in enhancing the efficacy of copper-based catalysts for CO_(2)RR,pointing towards a promising direction for the development of durable,high-performance electrocatalysts for sustainable chemical synthesis.
基金This work is supported by the National Key R&D Program of China(2021YFB3801600)the National Natural Science Foundation of China(22078005).
文摘Hydrogen peroxide(H_(2)O_(2))is a green oxidant that has been widely used.The direct synthesis of hydrogen peroxide(DSHP)offers significant advantages in terms of high atomic economy and environmentally friendly effects.However,due to the inevitable side reactions and severe mass transfer limitations,it is still challenging to balance the selectivity and activity for the DSHP.Combining theoretical understanding with the controllable synthesis of nanocatalysts may significantly facilitate the design of“dream catalysts”for the DSHP.In this work,the main factors affecting the reaction performance of catalysts and the active sites of catalysts have been reviewed and discussed in detail.The development and design of catalysts with high efficiency were introduced from three aspects:the catalyst support,active component and atomic impurity.In addition,the coupling of DSHP and other oxidation reactions to realize one-pot in situ oxidation reactions was comprehensively emphasized,which showed essential guiding significance for the future development of H_(2)O_(2).
基金Financial support from the National Natural Science Foundation of China(51773008,51533001,U1905217)the National Key Research and Development Program of China(2016YFC0801302)is gratefully acknowledged.
文摘Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their application as thermal interface materials.Herein,lamellarstructured polyamic acid salt/graphene oxide(PAAS/GO)hybrid aerogels are constructed by bidirectional freezing of PAAS/GO suspension followed by lyophilization.Subsequently,PAAS monomers are polymerized to polyimide(PI),while GO is converted to thermally reduced graphene oxide(RGO)during thermal annealing at 300℃.Final graphitization at 2800℃ converts PI to graphitized carbon with the inductive effect of RGO,and simultaneously,RGO is thermally reduced and healed to high-quality graphene.Consequently,lamellar-structured graphene aerogels with superior through-plane thermal conduction capacity are fabricated for the first time,and its superior through-plane thermal conduction capacity results from its vertically aligned and closely stacked high-quality graphene lamellae.After vacuum-assisted impregnation with epoxy,the resultant epoxy composite with 2.30 vol% of graphene exhibits an outstanding through-plane thermal conductivity of as high as 20.0 W m^−1 K^−1,100 times of that of epoxy,with a record-high specific thermal conductivity enhancement of 4310%.Furthermore,the lamellar-structured graphene aerogel endows epoxy with a high fracture toughness,~1.71 times of that of epoxy.
基金Supported by the National Natural Science Foundation of China(21676022,21706004)the Fundamental Research Funds for the Central Universities(BHYC1701A).
文摘In the present study,we propose a novel electrode material ofβ-nickel hydroxide covering nickel/aluminum layered double hydroxides via a facile complexation–precipitation method.The as-obtained materials with 3-dimensional nanostructures are further utilized as highly capable electrode material in nickel–metal hydride batteries.The electrochemical test results demonstrated theβ-nickel hydroxide covering nickel/aluminum-layered double hydroxides with 28%ofβ-nickel hydroxide provided a superior specific capacity value of 452 m A·h·g-1 in a current density of 5 A·g-1 using 6 M KOH as electrolyte as compared with other materials.In addition,the optimized sample displays an outstanding cyclic stability along with a huge specific capacity value of320 m Ah·g-1,and very small decay rate of 3.3%at 50 A·g-1 after 3000 cycles of charge/discharge test.These indicate that the newly designed material with nanostructures not only provides an efficient contact interface between electrolyte and active species and facilitates the transport of electrons and ions,but also protects the 3-dimensional nickel/aluminum layered double hydroxides,achieving a high specific capacity,fast redox reaction and excellent long-term cyclic stability.Therefore,theβ-nickel hydroxide covering nickel/aluminum layered double hydroxides with superior electrochemical performance is predictable to be a gifted electrode material in nickel–metal hydride batteries.
基金support from the National Natural Science Foundation of China(51922020,52090034)the Fundamental Research Funds for the Central Universities(BHYC1707B)。
文摘The highly integrated and miniaturized next-generation electronic products call for high-performance electromagnetic interference(EMI)shielding materials to assure the normal operation of their closely assembled components.However,the most current techniques are not adequate for the fabrication of shielding materials with programmable structure and controllable shielding efficiency.Herein,we demonstrate the direct ink writing of robust and highly conductive Ti3C2Tx MXene frames with customizable structures by using MXene/AlOOH inks for tunable EMI shielding and electromagnetic wave-induced thermochromism applications.The as-printed frames are reinforced by immersing in AlCl_(3)/HCl solution to remove the electrically insulating AlOOH nanoparticles,as well as cross-link the MXene sheets and fuse the filament interfaces with aluminum ions.After freeze-drying,the resultant robust and porous MXene frames exhibit tunable EMI shielding efficiencies in the range of 25-80 dB with the highest electrical conductivity of 5323 S m−1.Furthermore,an electromagnetic wave-induced thermochromic MXene pattern is assembled by coating and curing with thermochromic polydimethylsiloxane on a printed MXene pattern,and its color can be changed from blue to red under the high-intensity electromagnetic irradiation.This work demonstrates a direct ink printing of customizable EMI frames and patterns for tuning EMI shielding efficiency and visualizing electromagnetic waves.
基金Supported by the National Natural Science Foundation of China(21525625)the National Basic Research Program(973 Program) of China(2014CB745100)+3 种基金the(863) High Technology Project of China(2013AA020302)the Chinese Universities Scientific Fund(JD1417)China Postdoctoral Science Foundation funded project(2017M610038)the Fundamental Research Funds for the Central Universities(ZY1712,XK1701)
文摘Water pollution caused by highly toxic Cd(II), Pb(II), and Cr(VI) is a serious problem. In the present work,a green and low-cost adsorbent of g-C_3N_4 nanosheets was developed with superior capacity for both cationic and anionic heavy metals. The adsorbent was easily fabricated through one-step calcination of guanidine hydrochloride with thickness less than 1.6 nm and specific surface area of 111.2 m^2·g^(-1). Kinetic and isotherm studies suggest that the adsorption is an endothermic chemisorption process, occurring on the energetically heterogeneous surface based on a hybrid mechanism of multilayer and monolayer adsorption. The tri-s-triazine units and surface N-containing groups of g-C_3N_4 nanosheets are proposed to be responsible for the adsorption process.Further study on pH demonstrates that electrostatic interaction plays an important role. The maximum adsorption capacity of Cd(II), Pb(II), and Cr(VI) on g-C_3N_4 nanosheets is 123.205 mg·g^(-1), 136.571 mg·g^(-1),and 684.451 mg·g^(-1), respectively. The better adsorption performance of the adsorbent than that of the recently reported nanomaterials and low-cost adsorbents proves its great application potential in the removal of heavy metal contaminants from wastewater. The present paper developed a promising adsorbent which will certainly find applications in wastewater treatment and also provides guiding significance in designing adsorption processes.
基金supported by the National Natural Science Foundation of China (No. 51861165101)。
文摘Lithium-sulfur(Li-S) battery is one of the best candidates for the next-generation energy storage system due to its high theoretical capacity(1675 mA h-1),low cost and environment friendliness.However,lithium(Li) dendrites formation and polysulfide shuttle effect are two major challenges that limit the commercialization of Li-S batteries.Here we design a facile bifunctional interlayer of gelatin-based fibers(GFs),aiming to protect the Li anode surface from the dendrites growth and also hinder the polysulfide shuttle effect.We reveal that the 3D structural network of GFs layer with abundant polar sites helps to homogenize Li-ion flux,leading to uniform Li-ion deposition.Meanwhile,the polar moieties also immobilize the lithium polysulfides and protect the Li metal from the side-reaction.As a result,the anodeprotected batteries have shown significantly enhanced performance.A high coulombic efficiency of 96% after 160 cycles has been achieved in the Li-Cu half cells.The Li-Li symmetric cells exhibit a prolonged lifespan for 800 h with voltage hysteresis(10 mV).With the as-prepared GFs layer,the Li-S battery shows approximately 14% higher capacity retention than the pristine battery at 0.5 C after 100 cycles.Our work presents that this gelatin-based bi-functional interlayer provides a viable strategy for the manufacturing of advanced Li-S batteries.
基金supported by the National Key R&D Program(2017YFA0206804)the National Natural Science Foundation of China(21871021,21521005)the Fundamental Research Funds for the Central Universities(buctylkxj01,XK1802-6)~~
文摘Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al metal oxides(represented as Zn2ZrxAl-MMO)in light of the structural topotactic transformation of Zn2ZrxAl-hydrotalcite precursors(Zn2ZrxAl-LDH).The resulting Zn2ZrxAl-MMO catalysts were employed in the conversion of ethanol to diethyl carbonate.The Zr^4+ ion content of the LDH precursor plays a key role in modulating the acid-base properties and determining catalytic performance:the Zn2Zr0.1Al-MMO sample exhibits the optimal catalytic behavior with a diethyl carbonate(DEC)yield of 42.1%,which is the highest reported for metal oxide catalysts.Structure-property correlation investigations revealed that the synergic catalysis between medium-strong basic sites and weak acid sites plays a predominant role in the catalytic behavior.Furthermore,in situ Fourier transform infrared measurements showed that the weak acidic site promotes activation adsorption of the reactant(urea)and the intermediate product(ethyl carbamate),while the medium-strong basic site accelerates ethanol activation.Moreover,the Zn2Zr0.1Al-MMO catalyst has the advantages of cost effectiveness,good stability,and reusability.Therefore,the acid-base bifunctional catalysts developed in this work can be employed as promising candidates in acid-base catalytic reactions such as ethanol conversion.
文摘The synthesis of fluorescent nanomaterials has received considerable attention due to the great potential of these materials for a wide range of applications, from chemical sensing through bioimaging to optoelectron- ics. Herein, we report a facile and scalable approach to prepare fluorescent carbon dots (FCDs) via a one-pot reaction of citric acid with ethylenediamine at 150 ℃ under ambient air pressure. The resultant FCDs pos- sess an optical bandgap of 3.4 eV and exhibit strong excitation-wavelength-independent blue emission (λEm = 450 nm) under either one- or two-photon excitation. Owing to their low cytotoxicity and long fluorescence lifetime, these FCDs were successfully used as internalized fluorescent probes in human cancer cell lines (HeLa cells) for two-photon excited imaging of cells by fluorescence lifetime imaging microscopy with a high-contrast resolution. They were also homogenously mixed with commercial inks and used to draw fluo- rescent patterns on normal papers and on many other substrates (e.g., certain flexible plastic films, textiles, and clothes). Thus, these nanomaterials are promising for use in solid-state fluorescent sensing, security labeling, and wearable optoelectronics.
文摘C1 chemistry is the essence of coal chemistry and natural gas chemistry. Catalytic methods to efficiently convert C1 molecules into fuels and chemicals have been extensively studied. Syngas(CO +H_2) conversion is the most important industrial reaction system in C1 chemistry, and Fe and Co catalysts, two major industrial catalysts, have been the focus of fundamental research and industrial application. In the last decade, considerable research efforts have been devoted to discoveries concerning catalyst structure and increasing market demands for olefins and oxygenates. Since the development of efficient catalysts would strongly benefit from catalyst design and the establishment of a new reaction system, this review comprehensively overviews syngas conversion in three main reactions, highlights the advances recently made and the challenges that remain open, and will stimulate future research activities. The first part of the review summarizes the breakthroughs in Fischer-Tropsch synthesis regarding the optimization of activity and stability, determination of the active phase, and mechanistic studies. The second part overviews the modulation of catalytic structure and product selectivity for Fischer-Tropsch to olefins(FTO). Catalysts designed to produce higher alcohols, as well as to tune product selectivity in C1 chemistry, are described in the third section. Finally, present challenges in syngas conversion are proposed, and the solutions and prospects are discussed from the viewpoint of fundamental research and practical application. This review summarizes the latest advances in the design, preparation, and application of Fe/Co-based catalysts toward syngas conversion and presents the challenges and future directions in producing value-added fuels.
基金Financial support by the Fundamental Research Funds for the Central Universities(No.buctrc201727)the Natural Science Foundation of China(No.21536001,21722602,and 21322603)。
文摘Cost effective separation of acetylene(C_2H_2)and ethylene(C_2H_4)is of key importance to obtain essential chemical raw materials for polymer industry.Due to the low compression limit of C_2H_2,there is an urgent demand to develop suitable materials for efficiently separating the two gases under ambient conditions.In this paper,we provided a high-throughput screening strategy to study porous metal-organic frameworks(MOFs)containing open metal sites(OMS)for C_2H_2/C_2H_4 separation,followed by a rational design of novel MOFs in-silico.A set of accurate force fields was established from ab initio calculations to describe the critical role of OMS towards guest molecules.From a large-scale computational screening of 916 experimental Cu-paddlewheel-based MOFs,three materials were identified with excellent separation performance.The structure-performance relationships revealed that the optimal materials should have the largest cavity diameter around 5-10?and pore volume in-between 0.3-1.0 cm^3 g^(-1).Based on the systematic screening study result,three novel MOFs were further designed with the incorporation of fluorine functional group.The results showed that Cu-OMS and the-F group on the aromatic rings close to Cu sites could generate a synergistic effect on the preferential adsorption of C_2H_2 over C_2H_4,leading to a remarkable improvement of C_2H_2 separation performance of the materials.The findings could provide insight for future experimental design and synthesis of high-performance nanostructured materials for C_2H_2/C_2H_4 separation.
基金supported by the National Nature Science Foundation of China (U1707603, 21625101, 21521005, U1507102)the National Key Research and Development Program of China (2017YFB0307303)+2 种基金the 973 program (Grant No. 2014CB932104)Beijing Natural Science Foundation (2182047)the Fundamental Research Funds for the Central Universities (ZY1709)
文摘It is of significance to design of stable and cost-effective electrocatalyst for water splitting with high efficiency in an alkaline medium.The major obstacles for practical application of water splitting devices are lack of high-efficiency and low-cost electrocatalysts with low overpotential for both HER and OER.In this paper,we report a NiFe alloy decorated NiCoO2 hollow polyhedron(denoted as Ni Fe–Ni Co O2)by using[NiFe(CN)6]- intercalated NiCo–LDH as precursor.As evidenced by the electrochemical active surface area,the resultant Ni Fe–Ni Co O2 composite shows unique hollow nanostructure,which can not only provide abundant mass transport channels,but also increase the contact area of the NiFe–Ni Co O2 material with the electrolyte.The overpotential(η)demand is 286 mV for OER and 102 mV for HER at the current density of 10 mA/cm2 in an alkaline medium of 1 M KOH for the NiFe/NiCoO2 composite.This work provides a new pathway for preparation of the highly efficient bifunctional electrocatalysts for water splitting.
基金Project supported by the National Natural Science Foundation of China(Nos.61876059 and U1501251)
文摘An electronic-nose is developed based on eight quartz-crystal-microbalance (QCM) gas sensors in a sensor box, and is used to detect Chinese liquors at room temperature. Each sensor is a highly-accurate and highly-sensitive oscillator that has experienced airflow disturbances under the condition of varying room temperatures due to unstable flow-induced forces on the sensors surfaces. The three-dimensional (3D) nature of the airflow inside the sensor box and the interactions of the airflow on the sensors surfaces at different temperatures are studied by computational fluid dynamics (CFD) tools. Higher simulation accuracy is achieved by optimizing meshes, meshing the computational domain using a fine unstructural tetrahedron mesh. An optimum temperature, 30 ℃, is obtained by analyzing the distributions of velocity streamlines and the static pressure, as well as the flow-induced forces over time, all of which may be used to improve the identification accuracy of the electronic-nose for achieving stable and repeatable signals by removing the influence of temperature.
基金Supported by the National Natural Science Foundation of China(21676022)the Fundamental Research Funds for the Central Universities(BHYC170A&JD701)
文摘The present paper reports a new fluoride-free and energy-saving lead electrolytic refining process in order to solve the serious problems of the existing Betts lead electrorefining process, such as low production efficiency,high energy consumption and fluorine pollution. In the process, a mixed solution of perchloric acid and lead perchlorate(HClO4-Pb(ClO4)2) with the additives of gelatin and sodium lignin sulfonate is employed as the new electrolyte. The cathodic polarization curves show that HClO4 is very stable, and there is no any reduction reaction of HClO4 during the electrolytic process. The redox reactions of lead ions in HClO4 solution are very reversible with an ultrahigh capacity efficiency, so the HClO4 acts as a stable support electrolyte with higher ionic conductivity than the traditional H2SiF6 electrolyte. The results of the scale-up experiments show that under the optimal conditions of 2.8 mol·L-1 HClO4, 0.4 mol·L-1 Pb(ClO4)2 and electrolysis temperature of 45 ℃, the energy consumption is as low as 24.5 kW·h·(t Pb)-1 , only about 20% of that by Betts method at the same current density of 20 mA·cm-2, and the purity of the refined lead is up to 99.9992%, much higher than that specified by Chinese national standard(99.994%, GB/T 469-2013) and European standard(99.99%, EN 12659–1999).
基金Supported by the National Natural Science Foundation of China(21525625,21838001)the National Basic Research Program(973 Program)of China(2014CB745100)+1 种基金the(863)High Technology Project of China(2013AA020302)the Chinese Universities Scientific Fund(JD1417)
文摘Trace environmental pollutants have become a serious problem with special attention on the hazardous heavy metals, refractory organics, and pathogenic microorganisms. With coupling biosorption and photocatalysis to develop biomaterial/TiO2 composite photocatalysts is a promising method to remove these trace pollutants because of the synergistic effect. Biomaterials provide multiple function groups which can selectively and efficiently enrich trace pollutants onto the surface of the photocatalysts, thus facilitating the following transformation mediated by TiO2 photocatalysis. Biomaterials can also help the dispersion and recovery of TiO2, or even modify the band structure of TiO2. The fabrication of chitosan/TiO2, cellulose/TiO2, as well as other biomaterial/TiO2 composite photocatalysts is discussed in detail in this review. The application significance of these composite photocatalysts for the selective removal of trace pollutants is also addressed. Several problems should be solved before the realistic applications can be achieved as discussed in the final section.
基金supported by the National Natural Science Foundation of China(22005024,51873007,51961165102 and 21835006)。
文摘With advances in material science and a more in-depth understanding of device engineering,the power conversion efficiency(PCE)of solution-processed organic photovoltaic(OPV)cells have significantly boosted in the past few years.In 2019,a high PCE of 15.7%was achieved in the OPV cells adopting a wide bandgap polymer PM6 and a new emerging non-fullerene acceptor Y6.Such outstanding performance has attracted lots of research attention,driving considerable efforts to improve or take advantage of the high-performance PM6:Y6-based system.In this review,we first concentrate on the structural characteristics of PM6 and Y6 with the focus on understanding why their combination for OPV application can obtain such high efficiency.We also update the recent progress in highly efficient PM6:Y6-based OPV cells via various optimizing strategies.Then we summarize the other applications of the PM6:Y6-based system in semi-transparent,flexible or lay e-by-layer devices.The prospects for future OPV studies will be suggested in the end.
基金supported by National Natural Science Foundation of China,Beijing University of Chemical Technology(buctrc201901)National Natural Science Foundation of China and Ministry of Foreign A airs and International Cooperation,Italy(NSFC–MAECI 51861135202)+4 种基金the National Key Research and Development Project(Grant No.2018YFB1502401,2018YFA0702002)the Royal Society and the Newton Fund through the Newton Advanced Fellowship award(NAF\R1\191294)the Program for Changjiang Scholars and Innovation Research Team in the University(No.IRT1205)the Fundamental Research Funds for the Central Universitiesthe long–term subsidy mechanism from the Ministry of Finance and the Ministry of Education of PRC。
文摘Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction.Herein,atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery(termed as Fe-NSC) was synthesized,X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N3)(N-C-S).By enabling precisely localized S doping,the electronic structure of Fe-N4 moiety could be mediated,leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center.Density functional theory simulation suggested that more negative charge density would be localized over Fe-N4 moiety after S doping,allowing weakened binding capability to *OH intermediates and faster charge transfer from Fe center to O species.Electrochemical measurements revealed that the Fe-NSC sample exhibited significantly enhanced oxygen reduction reaction performance compared to the S-free Fe-NC material(termed as Fe-NC),showing an excellent onset potential of 1.09 V and half-wave potential of 0.92 V in 0.1 M KOH.Our work may enlighten relevant studies regarding to accessing improvement on the catalytic performance of atomically dispersed M-NC materials by managing precisely tuned local environments of M-Nx moiety.
文摘A precise understanding of the redox chemistry of Nm-Mn+(like N4-Fe^(2+))systems is essential for fundamental studies and rational design of Nm-Mn+-based electrocatalysts for the oxygen reduction reaction(ORR).Herein,three different iron phthalocyanines(FePcs)adsorbed on carbon nanotubes((NH2)4FePc@CNTs,(t-Bu)4FePc@CNTs,and FePc@CNTs)were evaluated to demonstrate the effect of the electron donating power of the substituents on the Fe^(3+)/Fe^(2+)redox potential of FePc@CNTs and the role of these composites as ORR mediators in alkaline media.The Fe^(3+)/Fe^(2+)redox potential of the FePcs was found to shift towards the cathodic region upon substitution with electron-donating groups.This up-field shift in the eg-orbital leads to a lower overlap between the onset potential of the Fe^(3+)/Fe^(2+)redox couple and that of the ORR,and thus,the ORR activity decreased in the following order based on the substitution of FePc:-H>-t-Bu>-NH2.
基金The authors acknowledge funding from the National Natural Science Foundation of China(61974150 and 51773213)Key Research Program of Frontier Sciences,CAS(QYZDB-SSW-JSC047)+1 种基金the Fundamental Research Funds for the Central Universities,the CAS-EU S&T cooperation partner program(174433KYSB20150013)the Natural Science Foundation of Ningbo(2018A610135).
文摘Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.