A hierarchically structured tin-cobalt composite with an enhanced electronic effect for high-performance CO_(2) electroreduction in a wide potential range

Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and formate.However,it is still difficult for Snbased materials to obtain satisfactory performance at low-to-moderate overpotentials.Herein,a simple and facile electrospinning technique is utilized to prepare a composite of a bimetallic Sn-Co oxide/carbon matrix with a hollow nanotube structure(Sn Co-HNT).Sn Co-HNT can maintain>90%faradaic efficiencies for C1 products within a wide potential range from-0.6 VRHE to-1.2 VRHE,and a highest 94.1%selectivity towards CO in an H-type cell.Moreover,a 91.2%faradaic efficiency with a 241.3 m A cm^(-2)partial current density for C1 products could be achieved using a flow cell.According to theoretical calculations,the fusing of Sn/Co oxides on the carbon matrix accelerates electron transfer at the atomic level,causing electron deficiency of Sn centers and reversible variation between Co^(2+)and Co^(3+)centers.The synergistic effect of the Sn/Co composition improves the electron affinity of the catalyst surface,which is conducive to the adsorption and stabilization of key intermediates and eventually increases the catalytic activity in CO_(2)electroreduction.This study could provide a new strategy for the construction of oxide-derived catalysts for CO_(2)electroreduction.

Fabrication and catalytic behavior of hierarchically-structured nylon 6 nanofiber membrane decorated with silver nanoparticles

A hierarchically‐structured nylon 6 (PA6) nanofiber membrane decorated with silver nanoparticles (Ag NPs) was fabricated by electrospinning and impregnation methods. The as‐fabricated hierarchically‐structured Ag/PA6 nanofiber membrane (HS‐Ag/PA6 NM) exhibits a morphology in which Ag NPs are deposited on the surfaces of both thick fibers and thin fibers. The content and size of theAg NPs can be controlled by varying the concentration of the silver colloid solution. Compared with the non‐hierarchically‐structured Ag/PA6 nanofiber membrane, HS‐Ag/PA6 NM has a higher specificsurface area and exhibits a higher degradation rate for methylene blue of 81.8%–98.1% within2 h. HS‐Ag/PA6 NM can be easily recycled and exhibits good reusability. It retains a degradation rate for methylene blue of 83.5% after five consecutive cycles. The hierarchically‐structured nanofiber membrane is therefore a potential nanocatalyst.

Self-supporting and hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as a bifunctional electrocatalyst for fluctuating overall water splitting

Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as bifunctional electrocatalyst was constructed based on porous Ni-Fe electrodeposition on three-dimensional(3D)carbon fiber cloth,in situ oxidation,and chemical sulfuration.Results showed that the Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)because of the abundance of active sites,synergistic effect of the heterostructure,superhydrophilic surface,and stable,self-supporting structure.The results further confirmed that the Ni_(x)Fe-S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni_(3)S_(2) during OER.Compared with the commercial 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer,the self-supporting Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) electrolyzer exhibits better stability and lower cell voltage in the fluctu-ating current density range of 10-500 mA/cm^(2).Particularly,the cell voltage of Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) is only approximately 3.91 V at an industrial current density of 500 mA/cm^(2),which is lower than that of the 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer(i.e.,approximately 4.79 V).This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.

Nitrogen and sulfur co-doped graphene aerogel with hierarchically porous structure for high-performance supercapacitors

Supercapacitors with unique performance have been widely utilized in many fields. Herein, we report a nitrogen and sulfur co-doped graphene aerogel(N/S-GA-2) prepared using a low toxic precursor for high-performance supercapacitors. The as-obtained material possesses a hierarchically porous structure and a large number of electrochemical active sites. At a current density of 1 Ag^-1, the specific capacitance of the N/S-GA-2 for supercapacitors with the ionic liquid as the electrolyte is 169.4 Fg^-1, and the corresponding energy density is 84.5 Wh kg^-1.At a power density of 8.9 k W kg^-1, the energy density can reach up to 75.7 Wh kg^-1, showing that the N/S-GA-2 has an excellent electrochemical performance. Consequently, the N/S-GA-2 can be used as a promising candidate of electrode materials for supercapacitors with high power density and high energy density.

Self-template synthesis of hierarchically structured Co3O4@NiO bifunctional electrodes for selective nitrate reduction and tetrahydroisoquinolines semidehydrogenation

The rational design and synthesis of hierarchically hollow nanostructures with controlled spatial architecture and composition are significant in electrocatalysis owing to their abundant active sites and the expedited electron/mass transfer.Electrocatalytic nitrate reduction to ammonia is of great interest from the points of environmental protection and energy saving.However,the development of this technology is hindered by the lack of efficient nitrate-toammonia electrocatalysts and the kinetically sluggish oxygen evolution reaction at the anode.Herein,a novel self-template conversion method was developed for the synthesis of Co3O4@Ni O hierarchical nanotubes(Co3O4@Ni O HNTs)with Ni O porous nanosheets assembled on Co3O4nanotubes.The as-obtained Co3O4@Ni O HNTs exhibited an outstanding performance for both the cathodic nitrate electroreduction to ammonia reaction and the anodic tetrahydroisoquinolines(THIQs)semi-dehydrogenation to dihydroisoquinolines(DHIQs).Importantly,a two-electrode system of Co3O4@Ni O HNTs||Co3O4@Ni O HNTs was constructed for the simultaneous synthesis of ammonia and DHIQs with high selectivity and robust stability.

Hierarchically structured flower-like Ru nanoparticles-cucurbit[6]uril/multiwalled carbon nanotubes as efficient pH-universal hydrogen evolution electrocatalyst

Developing efficient and stable electrocatalyst to hydrogen evolution reaction adaptable for electrolytes with different p H is a big challenge.In this work,a hierarchically structured ternary nanohybrid composed of flower-like Ru nanoparticles,rigid macrocyclic cucurbit[6]uril(CB[6])and carboxylated multiwalled carbon nanotubes(MWCNTs)was successfully prepared by chemical wet method.Benefited by the structural merits of flower-like Ru nanoparticles exposed abundant active sites supported by the MWCNTs holding superior mass transport and electrons transfer ability as well as the existence of CB[6],the obtained catalyst exhibited outstanding HER activities with overpotentials of 27,37 and 70 m V at-10 m A/cm^(2) in alkaline,acidic,and neutral electrolytes,respectively.Under the same electrocatalytic operation conditions,the HER performance is comparable or superior to commercial Pt/C catalyst(47,27and 49 m V).Besides,chronopotentiometric and accelerated stability test also revealed its extraordinary stability,which could be further employed for electrocatalytic procedure in a broad pH range.

Boosting ethanol oxidation over nickel oxide through construction of quasi-one-dimensional morphology and hierarchically porous structure

Quasi-one-dimensional NiO with a hierarchically porous structure was synthesized through a facile coordination−precipitation method with the coupling effect of ammonia and a post-calcination treatment.The electrocatalytic properties of NiO fibers for the oxidation of ethanol were compared with those of NiO spheres.The results show that the fibrous NiO possesses a larger specific surface area of 140.153 m2/g and a lower electrical resistivity of 4.5×105Ω·m,leading to an impressively superior electrocatalytic activity to spherical NiO for ethanol oxidation in alkaline media.The current decay on fibrous NiO at 0.6 V in 100−900 s was 0.00003%,which is much lower than that of spherical NiO,indicating its better stability.The unique morphology and hierarchically porous structure give the fibrous NiO great potential to be used as an anodic electrocatalyst for direct ethanol fuel cells.

Hierarchically Structured Three-Dimensional Carbon-Based Integrated Electrodes with Enhanced Pseudocapacitance and Deformability

Compressible supercapacitors play an increasingly significant role in flexible sensors and wearable electronic devices.However,the integration of mechanical compressibility and excellent electrochemical performance into a single device remains a challenge.Herein,we demonstrate a compressible and high-performance supercapacitor based on an N-doped carbon foam elastomer with hierarchical carbon nanotubes.Hierarchically structured Fe3C@N-doped carbon nanotubes/N-doped carbon foam and Ni@N-doped carbon nanotubes/N-doped carbon foam have been synthesized via a simple and universal self-catalytic strategy.The hierarchical structural features of self-catalytic N-doped carbon nanotubes serve as a cushion when the composite is subjected to an external force,exhibiting excellent mechanical properties with a maximum compressive strain of 80%and fatigue resistance of 1000 cycles.Moreover,the different electroactive potentials of the transition-metal species in the composites provide the assembly with a maximum operating voltage of 1.4 V,which shows a maximum energy density of∼10.74 Wh kg^(−1)(0.084 mWh cm^(−3))at the power density of∼179.2 W kg^(−1)(1.4 mWh cm^(−3)),and retains 88.4%of the original capacitance after 20,000 charge–discharge cycles,even at a strain of 80%.This work paves the way for controllable fabrication of compressible electrodes and supercapacitors.

Hierarchical structures on platinum-iridium substrates enhancing conducting polymer adhesion

Conducting polymers(CPs),including poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS),are promising coating materials for neural electrodes.However,the weak adhesion of CP coatings to substrates such as platinum-iridium is a significant challenge that limits their practical application.To address this issue,we used femtosecond laser-prepared hierarchical structures on platinum-iridium(Pt-Ir)substrates to enhance the adhesion of PEDOT:PSS coatings.Next,we used cyclic voltammetry(CV)stress and accelerated aging tests to evaluate the stability of both drop cast and electrodeposited PEDOT:PSS coatings on Pt-Ir substrates,both with and without hierarchical structures.Our results showed that after 2000 CV cycles or five weeks of aging at 60℃,the morphology and electrochemical properties of the coatings on the Pt-Ir substrates with hierarchical structures remained relatively stable.In contrast,we found that smooth Pt-Ir substrate surfaces caused delamination of the PEDOT:PSS coating and exhibited both decreased charge storage capacity and increased impedance.Overall,enhancing the stability of PEDOT:PSS coatings used on common platinum-iridium neural electrodes offers great potential for improving their electrochemical performance and developing new functionalities.

Achieving the synergistic of strength and ductility in Mg-15Gd-1Zn-0.4Zr alloy with hierarchical structure

Currently,the hierarchical structure is one of the most effective means to enhance the strength and plasticity of metal materials,since the strain localization can be effectively delayed by the coordination of the unique microstructure.In this study,a hierarchical structure of Mg-15Gd-1Zn-0.4Zr(GZ151K)alloys containing grain,twin,and precipitation structural units was prepared by ultrasonic surface rolling process(USRP)and recrystallization annealing(RU).The results showed that the stress gradient generated by USRP formed a twin gradient structure,which will activate the twin-assisted precipitation(TAP)effect and twin-induced recrystallization(TIR)effect during RU.Then,the twin gradient structure transformed into a twin-precipitation gradient structure,and finally into a hierarchical structure with grain-twinprecipitation as the increasement of recrystallization degree.Besides,the dual gradient structure with twin and precipitation structural units had the highest strength and microhardness owing to the precipitation strengthening.However,the hierarchical structure with grain,twin,and precipitation structural units exhibited the most excellent combination of strength and plasticity under grain refinement and precipitation strengthening.

Remarkably Enhanced Methane Sensing Performance at Room Temperature via Constructing a Self-Assembled Mulberry-Like ZnO/SnO_(2) Hierarchical Structure

Development of metal oxide semiconductors-based methane sensors with good response and low power consumption is one of the major challenges to realize the real-time monitoring of methane leakage.In this work,a self-assembled mulberry-like ZnO/SnO_(2)hierarchical structure is constructed by a two-step hydrothermal method.The resultant sensor works at room temperature with excellent response of~56.1%to 2000 ppm CH_(4)at 55%relative humidity.It is found that the strain induced at the ZnO/SnO_(2)interface greatly enhances the piezoelectric polarization on the ZnO surface and that the band bending results in the accumulation of chemically adsorbed O_(2)^(-)ions close to the interface,leading to significant improvement in the sensing performance of the methane gas sensor at room temperature.

Nano-Au-decorated hierarchical porous cobalt sulfide derived from ZIF-67 toward optimized oxygen evolution catalysis:Important roles of microstructures and electronic modulation

Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.

Effects of hierarchical structure on the performance of tin oxide-supported platinum catalyst for room-temperature formaldehyde oxidation

Flower-like tin oxide-supported platinum（Pt/SnOx） with a hierarchical structure was synthesized by a hydrothermal method and characterized by XRD,SEM,TEM,high resolution TEM,XPS and nitrogen adsorption.The flower-like Pt/SnOx microspheres of 1 μm in diameter were composed of staggered petal-like nanosheets with a thickness of 20 nm.Pt nanoparticles（NPs） of 2-3 nm were well dispersed on the SnOx nanosheets.The catalyst was tested in the catalytic oxidation of gaseous formaldehyde（HCHO） at room temperature,and exhibited enhanced activity compared to Pt NPs supported on commercial SnO and ground SnOx.HCHO removal of 87%was achieved over the hierarchical Pt/SnOx after 1 h of reaction,which was 1.5 times that over the ground SnOx-supported Pt（Pt/g-SnOx）,and the high activity was maintained after six recycles,showing the high stability of this catalyst.HCHO decomposition kinetics was modeled as a second order reaction.The reaction rate constant for Pt/SnOx was 5.6 times higher than Pt/g-SnOx.The hierarchical pore structure was beneficial for the diffusion and adsorption of HCHO molecules,and the highly dispersed Pt NPs on the SnOx nanosheets were the active sites for the oxidative decomposition of HCHO into CO2 and H2O.This study provided a promising approach for designing efficient catalysts for indoor HCHO removal at ambient temperature.

Plant Surfaces:Structures and Functions for Biomimetic Innovations

An overview of plant surface structures and their evolution is presented. It combines surface chemistry and architecture with their functions and refers to possible biomimetic applications. Within some 3.5 billion years biological species evolved highly complex multifunctional surfaces for interacting with their environments: some 10 million living prototypes(i.e., estimated number of existing plants and animals) for engineers. The complexity of the hierarchical structures and their functionality in biological organisms surpasses all abiotic natural surfaces: even superhydrophobicity is restricted in nature to living organisms and was probably a key evolutionary step with the invasion of terrestrial habitats some 350–450 million years ago in plants and insects. Special attention should be paid to the fact that global environmental change implies a dramatic loss of species and with it the biological role models. Plants, the dominating group of organisms on our planet, are sessile organisms with large multifunctional surfaces and thus exhibit particular intriguing features.Superhydrophilicity and superhydrophobicity are focal points in this work. We estimate that superhydrophobic plant leaves(e.g., grasses) comprise in total an area of around 250 million km^2, which is about 50% of the total surface of our planet. A survey of structures and functions based on own examinations of almost 20,000 species is provided, for further references we refer to Barthlott et al.(Philos. Trans. R. Soc. A 374: 20160191, 1). A basic difference exists between aquatic nonvascular and land-living vascular plants; the latter exhibit a particular intriguing surface chemistry and architecture. The diversity of features is described in detail according to their hierarchical structural order. The first underlying and essential feature is the polymer cuticle superimposed by epicuticular wax and the curvature of single cells up to complex multicellular structures. A descriptive terminology for this diversity is provided. Simplified, the functions of plant surface characteristics may be grouped into six categories:(1) mechanical properties,(2) influence on reflection and absorption of spectral radiation,(3) reduction of water loss or increase of water uptake, moisture harvesting,(4) adhesion and nonadhesion(lotus effect, insect trapping),(5) drag and turbulence increase, or(6) air retention under water for drag reduction or gas exchange(Salvinia effect). This list is far from complete. A short overview of the history of bionics and the impressive spectrum of existing and anticipated biomimetic applications are provided. The major challenge for engineers and materials scientists, the durability of the fragile nanocoatings, is also discussed.

Integration of Multiple Heterointerfaces in a Hierarchical 0D@2D@1D Structure for Lightweight,Flexible,and Hydrophobic Multifunctional Electromagnetic Protective Fabrics

The development of wearable multifunctional electromagnetic protective fabrics with multifunctional,low cost,and high efficiency remains a challenge.Here,inspired by the unique flower branch shape of“Thunberg’s meadowsweet”in nature,a nanofibrous composite membrane with hierarchical structure was constructed.Integrating sophisticated 0D@2D@1D hierarchical structures with multiple heterointerfaces can fully unleash the multifunctional application potential of composite membrane.The targeted induction method was used to precisely regulate the formation site and morphology of the metal–organic framework precursor,and intelligently integrate multiple heterostructures to enhance dielectric polarization,which improves the impedance matching and loss mechanisms of the electromagnetic wave absorbing materials.Due to the synergistic enhancement of electrospinning-derived carbon nanofiber“stems”,MOF-derived carbon nanosheet“petals”and transition metal selenide nano-particle“stamens”,the CoxSey/NiSe@CNSs@CNFs(CNCC)composite membrane obtains a minimum reflection loss value(RL_(min))of-68.40 dB at 2.6 mm and a maximum effective absorption bandwidth(EAB)of 8.88 GHz at a thin thickness of 2.0 mm with a filling amount of only 5 wt%.In addition,the multi-component and hierarchical heterostructure endow the fibrous membrane with excellent flexibility,water resistance,thermal management,and other multifunctional properties.This work provides unique perspectives for the precise design and rational application of multifunctional fabrics.

A Novel Hierarchical Porous 3D Structured Vanadium Nitride/Carbon Membranes for High-performance Supercapacitor Negative Electrodes

Transition-metal nitrides exhibit wide potential windows and good electrochemical performance, but usually experience imbalanced practical applications in the energy storage field due to aggregation, poor circulation stability, and complicated syntheses. In this study, a novel and simple multiphase polymeric strategy was developed to fabricate hybrid vanadium nitride/carbon(VN/C) membranes for supercapacitor negative electrodes, in which VN nanoparticles were uniformly distributed in the hierarchical porous carbon 3D networks. The supercapacitor negative electrode based on VN/C membranes exhibited a high specific capacitance of 392.0 F g^(-1) at 0.5 A g^(-1) and an excellent rate capability with capacitance retention of 50.5% at 30 A g^(-1). For the asymmetric device fabricated using Ni(OH)_2//VN/C membranes, a high energy density of 43.0 Wh kg^(-1) at a power density of800 W kg^(-1) was observed. Moreover, the device also showed good cycling stability of 82.9% at a current density of 1.0 A g^(-1) after 8000 cycles. This work may throw a light on simply the fabrication of other high-performance transition-metal nitridebased supercapacitor or other energy storage devices.

Hierarchically porous nitrogen-doped carbon as cathode for lithium–sulfur batteries

Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon （HPNC） via acombination of salt template （ZnC12） and hard template （SiO2） as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC （IC= 1675 mAh g^-1 ）, a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.

High-performance all-solid-state polymer electrolyte with fast conductivity pathway formed by hierarchical structure polyamide 6 nanofiber for lithium metal battery

The utilization of all-solid-state electrolytes is considered to be an effective way to enhance the safety performance of lithium metal batteries.However,the low ionic conductivity and poor interface compatibility greatly restrict the development of all-solid-state battery.In this study,a composite electrolyte combining the electrospun polyamide 6(PA6)nanofiber membrane with hierarchical structure and the polyethylene oxide(PEO)polymer is investigated.The introduction of PA6 nanofiber membrane can effectively reduce the crystallinity of the polymer,so that the ionic conductivity of the electrolyte can be enhanced.Moreover,it is found that the presence of finely branched fibers in the hierarchical structure PA6 membrane allows the polar functional groups(C=O and N-H bonds)to be fully exposed,which provides sufficient functional sites for lithium ion transport and helps to regulate the uniform deposition of lithium metal.Moreover,the hierarchical structure can enhance the mechanical strength(9.2 MPa)of the electrolyte,thereby effectively improving the safety and cycle stability of the battery.The prepared Li/Li symmetric battery can be stably cycled for 1500 h under 0.3 mA cm^(-2) and 60℃.This study demonstrates that the prepared electrolyte has excellent application prospects in the next generation all-solid-state lithium metal batteries.

Hierarchical structure observation and nanoindentation size effect characterization for a limnetic shell

In the present research, hierarchical structure observation and mechanical property characterization for a type of biomaterial are carried out. The investigated bioma- terial is Hyriopsis cumingii, a typical limnetic shell, which consists of two different structural layers, a prismatic ＂pillar＂ structure and a nacreous ＂brick and mortar＂ structure. The prismatic layer looks like a ＂pillar forest＂ with variationsection pillars sized on the order of several tens of microns. The nacreous material looks like a ＂brick wall＂ with bricks sized on the order of several microns. Both pillars and bricks are composed of nanoparticles. The mechanical properties of the hierarchical biomaterial are measured by using the nanoindentation test. Hardness and modulus are measured for both the nacre layer and the prismatic layer, respectively. The nanoindentation size effects for the hierarchical structural materials are investigated experimentally. The results show that the prismatic nanostructured material has a higher stiffness and hardness than the nacre nanostructured material. In addition, the nanoindentation size effects for the hierarchical structural materials are described theoretically, by using the trans-scale mechanics theory considering both strain gradient effect and the surface/interface effect. The modeling results are consistent with experimental ones.

Hierarchical Carbon Microtube@Nanotube Core-Shell Structure for High-Performance Oxygen Electrocatalysis and Zn-Air Battery

Zinc-air batteries(ZABs)hold tremendous promise for clean and efficient energy storage with the merits of high theoretical energy density and environmental friendliness.However,the performance of practical ZABs is still unsatisfactory because of the inevitably decreased activity of electrocatalysts when assembly into a thick electrode with high mass loading.Herein,we report a hierarchical electrocatalyst based on carbon microtube@nanotube core-shell nanostructure(CMT@CNT),which demonstrates superior electrocatalytic activity for oxygen reduction reaction and oxygen evolution reaction with a small potential gap of 0.678 V.Remarkably,when being employed as air-cathode in ZAB,the CMT@CNT presents an excellent performance with a high power density(160.6 mW cm^−2),specific capacity(781.7 mAhgZn^−1)as well as long cycle stability(117 h,351 cycles).Moreover,the ZAB performance of CMT@CNT is maintained well even under high mass loading(3 mg cm−2,three times as much as traditional usage),which could afford high power density and energy density for advanced electronic equipment.We believe that this work is promising for the rational design of hierarchical structured electrocatalysts for advanced metal-air batteries.