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能源与环境材料(英文)
能源与环境材料(英文)
能源与环境材料(英文)/Journal Energy & Environmental MaterialsSCI
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    Isolated Co Atoms Anchored on Defective Nitrogen-doped Carbon Graphene as Efficient Oxygen Reduction Reaction Electrocatalysts

    Peng RaoJunming LuoDaoxiong WuJing Li...
    239-244页
    查看更多>>摘要:Oxygen reduction reaction(ORR)is the heart of many new energy conversions and storage devices,such as metal-air batteries and fuel cells.However,ORR is currently facing the dilemma of sluggish intrinsic kinetics and the noble electrocatalysts of high price and low reserves.In this work,isolated Co atoms anchored on defective nitrogen-doped carbon graphene single-atom catalyst(Co-SAC/NC)are synthesized via the proposed movable type printing method.The prepared Co-SAC/NC catalyst demonstrates admirable ORR performance,with a high half-wave potential of 0.884 V in alkaline electrolytes and outstanding durability.In addition,an assembled zinc-air battery with prepared Co-SAC/NC as air-cathode catalyst displays a high-peak power density of 179 mW cm-2 and a high-specific capacity(757 mAh g-1).Density functional theory calculations confirm that the true active sites of the prepared catalyst are Co-N4 moieties,and further reveal a significantly electronic structure evolution of Co sites in the ORR process,in which the project density of states and local magnetic moment of Co atom varies during its whole reaction process.This work not only paves a new avenue for synthesizing SACs as robust electrocatalysts,but also provides an electronic-level insight into the evolution of the electronic structure of single-atom catalysts.

    Growing Biomorphic Transition Metal Dichalcogenides and Their Alloys Toward High Permeable Membranes and Efficient Electrocatalysts Applications

    Lijie ZhuYahuan HuanZhaoqian ZhangPengfei Yang...
    245-255页
    查看更多>>摘要:3D architecratured transition metal dichalcogenides constructed by atomically thin layers are appealing building blocks in various applications,such as catalysts,energy storage,conversions,sensors,and so on.However,the direct growth of 3D transition metal dichalcogenides architectures with high crystal quality and well-controlled size/thickness remains a huge challenge.Herein,we report a facile,highly-repeatable,and versatile chemical vapor deposition strategy,for the mass production of high-quality 3D-architecratured transition metal dichalcogenides(e.g.,MoS2,WS2,and ReS2)and their alloys(e.g.,WxMo(1-x)S2 and RexMo(1-x)S2)nanosheets on naturally abundant and low-cost diatomite templates.Particularly,the purified transition metal dichalcogenides products exhibit unique and designable 3D biomorphic hierarchical microstructures,controllable layer thicknesses,tailorable chemical compositions,and good crystallinities.The weak interlayer interactions endow them with good dispersity in solutions to form stable additive-free inks for solution-processing-based applications,for example,high-permeable and high-stable separation membranes for water purification,and efficient electrocatalysts for hydrogen evolution reactions.This work paves ways for the low-cost,mass production of versatile transition metal dichalcogenides powder-like materials with designable structures and properties,toward energy/environmental-related applications and beyond.

    Three-Dimensional N-Doped Carbon Nanotube/Graphene Composite Aerogel Anode to Develop High-Power Microbial Fuel Cell

    Shixuan JinYiyu FengJichao JiaFulai Zhao...
    256-264页
    查看更多>>摘要:Optimizing the structure of electrode materials is one of the most effective strategies for designing high-power microbial fuel cells(MFCs).However,electrode materials currently suffer from a series of shortcomings that limit the output of MFCs,such as high intrinsic resistance,poor electrolyte wettability,and low microbial load capacity.Here,a three-dimensional(3D)nitrogen-doped multiwalled carbon nanotube/graphene(N-MWCNT/GA)composite aerogel is synthesized as the anode for MFCs.Comparing nitrogen-doped GA,MWCNT/GA,and N-MWCNT/GA,the macroporous hydrophilic N-MWCNT/GA electrode with an average pore size of 4.24 pm enables high-density loading of the microbes and facilitates extracellular electron transfer with low intrinsic resistance.Consequently,the hydrophilic surface of N-MWCNT can generate high charge mobility,enabling a high-power output performance of the MFC.In consequence,the MFC system based on N-MWCNT/GA anode exhibits a peak power density and output voltage of 2977.8 mW m-2 and 0.654 V,which are 1.83 times and 16.3%higher than those obtained with MWCNT/GA,respectively.These results demonstrate that 3D N-MWCNT/GA anodes can be developed for high-power MFCs in different environments by optimizing their chemical and microstructures.

    High-Throughput Pb Recycling for Perovskite Solar Cells Using Biomimetic Whitlockite

    Jung Sug HongHee Jung KimChang Hwun SohnOh Yeong Gong...
    265-271页
    查看更多>>摘要:Pb contamination in aquatic environments causes severe pollution;therefore,harmless absorbents are required.In this study,we report a novel synthesis of whitlockite(WH,Ca18Mg2(HPO4)2(PO4)12),which is the second most abundant biomineral in human bone,and its application as a high-performing Pb2+absorbent.Hydroxyapatite(HAP)and WH are prepared via a simple precipitation method.The Pb2+absorption performance and mechanism of the synthesized biominerals are investigated in aqueous solutions at neutral pH.The results demonstrate that WH exhibits an excellent Pb2+absorption capacity of 2339 mg g-1,which is 1.68 times higher than the recorded value for HAP.Furthermore,the absorbed Pb2+ions are recycled into high-purity Pbl2.This is employed as a precursor for the fabrication of perovskite solar cells(PSCs),resulting in a conversion efficiency of 19.00%comparable to that of commercial Pbl2 powder(99.99%purity).Our approach provides an efficient way to remove Pb2+ions from water and reuse them in the recycling of PSCs.

    Construction of 3D Shape-Changing Hydrogels via Light-Modulated Internal Stress Fields

    Zihan XuWenxin FanJinghua DuanYanzhi Xia...
    272-278页
    查看更多>>摘要:The 3D shape-changing hydrogels are highly pursued for numerous applications.However,up to now,the construction of complex 3D shape-changing hydrogels remains a challenge.The reported design strategies are mainly applied to fabricate 2D ones by introducing anisotropic microstructures into hydrogel sheets/membranes.Herein,we present a convenient photolithography strategy for constructing complex 3D shape-changing hydrogels by simultaneously modulating anisotropic microstructures and internal stress fields of gel sheets.When the precursor solution containing ultraviolet(UV)absorber is irradiated by single-side UV light,the attenuated polymerization rate can cause the generation of asymmetric internal stress field in the resulting hydrogel sheet.In the meantime,the directional diffusion of unpolymerized monomers allows for the formation of vertical gradient structure within hydrogel.Therefore,by applying different photomasks to modulate the local gradient structures and internal stress fields of the gel sheets,they can spontaneously transform into various complex 3D shape-changing hydrogels in the air.Response to the external stimuli,these 3D shape-changing hydrogels(e.g.,fighter plane,birdie,and multi-storey origami lattices)can deform in a novel 3D1-to-3D2-to-3D3 mode.This new design strategy contributes to the development of complex biomedical implants and soft robotics.

    Simultaneous Solar-driven Steam and Electricity Generation by Cost-effective,Easy Scale-up MnO2-based Flexible Membranes

    Jiaxin RenYang DingJiang GongJinping Qu...
    279-287页
    查看更多>>摘要:Harvesting solar energy in an effective manner for steam and electricity generation is a promising technique to simultaneously cope with the energy and water crises.However,the construction of efficient and easy scale-up photothermal materials for steam and electricity cogeneration remains challenging.Herein,we report a facile and cost-effective strategy to prepare MnO2-decorated cotton cloth(MCx).The wide adsorption spectrum and excellent photothermal conversion ability of the in situ-formed MnO2 nanoparticles make the MCx to be advanced photothermal materials.Consequently,the hybrid device integrated with MCx as the photothermal layer and the thermoelectric(TE)module for electricity power conversion exhibits an extremely high evaporation rate of 2.24 kg m-2 h-1 under 1 kW m-2 irradiation,which is ranked among the most powerful solar evaporators.More importantly,during solar evaporation,the hybrid device produces an open-circuit voltage of 0.3 V and a power output of 1.6 W m-2 under 3 Sun irradiation,and outperforms most of the previously reported solar-driven electricity generation devices.Therefore,the integrated device with synergistic solar-thermal utilization opens up a green way toward simultaneous solar vapor and electric power generation in remote and resource-constrained areas.

    Create Rich Oxygen Defects of Unique Tubular Hierarchical Molybdenum Dioxide to Modulate Electron Transfer Rate for Superior High-Energy Metal-Ion Hybrid Capacitor

    Heng ZhangJinggao WuZhuo ZouYoucun Bai...
    288-299页
    查看更多>>摘要:Metal-ion capacitors could merit advantages from both batteries and capacitors,but they need to overcome the severe restrictions from their sluggish reaction kinetics of the battery type electrode and low specific capacitance of capacitor type electrode for both high energy and power density.Herein,we use the Kirkendall effect for the first time to synthesize unique tubular hierarchical molybdenum dioxide with encapsulated nitrogen-doped carbon sheets while in situ realizing phosphorus-doping to create rich oxygen vacancies(P-MoO2.x@NP-C)as a sodium-ion electrode.Experimental and theoretical analysis confirm that the P-doping introduced oxygen defects can partially convert the high-bond-energy Mo-O to low-bond-energy Mo-P,resulting in a low oxidation state of molybdenum for enhanced surface reactivity and rapid reaction kinetics.The as-prepared P-MoO2.x@NP-C as an ion-battery electrode is further used to pair active N-doped carbon nanosheet(N-C-A)electrode for Na-ion hybrid capacitor,delivering excellent performance with an energy density of 140.3 Wh kg-1,a power density of 188.5 W kg-1 and long stable life in non-aqueous solution,which ranks the best among all reported MoOx-based hybrid capacitors.P-MoO2.x@NP-C is also used to fabricate a zinc-ion hybrid capacitor,also accomplishing a remarkable energy density of 43.8 Wh kg-1,a power density of 93.9 W kg-1,and a long stable life@2A g-1 of 32 000 cycles in aqueous solutions,solidly verifying its universal significance.This work not only demonstrates an innovative approach to synthesize high-performance metal ion hybrid capacitor materials but also reveals certain scientific insights into electron transfer enhancement mechanisms.

    Unraveling the Role of Nitrogen-Doped Carbon Nanowires Incorporated with MnO2 Nanosheets as High Performance Cathode for Zinc-Ion Batteries

    Xiaohui LiQiancheng ZhouZe YangXing Zhou...
    300-308页
    查看更多>>摘要:Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO2 for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO2 with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO2@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO2@NC electrode shows an enhanced specific capacity(325 mAh g-1 at 0.1 A g-1)and rate performance(90 mAh g-1 at 2 A g-1),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO2 incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn4+ion in MnO2 crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn2+/H+insert into the host MnO2 lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials.

    Non-Fullerene-Based Inverted Organic Photovoltaic Device with Long-Term Stability

    Do Hui KimFebrian T.A.WibowoDongchan LeeNarra V.Krishna...
    309-316页
    查看更多>>摘要:In this work,we developed the PM6:Y6-based inverted structure organic photovoltaic(i-OPV)with improved power conversion efficiency(PCE)and long-term stability by resolving the origins of the performance deterioration.The deep defects between the metal oxide-based electron transport layer and bulk-heterojunction photoactive layer interface were responsible for suboptimal PCE and facilitated degradation of devices.While the density of deep traps is increased during the storage of i-OPV,the penetrative oxygen-containing defects additionally generated shallow traps below the band-edge of Y6,causing an additional loss in the open-circuit voltage.The suppression of interfacial defects by chemical modification effectively improved the PCE and long-term stability of i-OPV.The modified i-OPV(mi-OPV)achieved a PCE of 17.42%,which is the highest value among the reported PM6:Y6-based i-OPV devices.Moreover,long-term stability was significantly improved:~90%and~80%retention of its initial PCE after 1200 h of air storage and illumination,respectively.

    Jahn-Teller Effect Directed Bandgap Tuning of Birnessite for Pseudocapacitive Application

    Sheng ZhuYuechao WangJinshu ZhangJian Sheng...
    317-323页
    查看更多>>摘要:Birnessite MxMnO2(M=Na+,K+,etc.)has emerged as a promising alternative to the classical MnO2 material owing to its improved pseudocapacitive performance for energy storage.Understanding their structure-property correlation is essential for the development and application of advanced supercapacitors.Herein,we adopt the crystal field theory and density functional simulation to reveal the structural dependence of the pseudocapacitive property of KxMnO2.Attributing to the Jahn-Teller effect of Mn3+,the bandgap of KxMnO2 can be tuned by changing the x value(i.e.,the Mn(Ⅲ)/Mn(Ⅳ)ratio).Then,we design a narrow-bandgap K0.25MnO2(0.84 eV),which affords a high capacitance of 415 F g-1 at 1 A g-1 and a desirable rate capability of 293 F g-1 at 20 A g-1.Operando Raman spectroscopy confirms that the Jahn-Teller induced structure evolution of[MnO6]octahedron accounts for the superior pseudocapacitive behavior of K0.25MnO2.This finding offers theoretical guidance to the design and application of birnessite materials for pseudocapacitors.