Global band convergence design for high-performance thermoelectric power generation in Zintls.

Electronic band convergence can have a beneficial impact on thermoelectric performance, but finding the right band-converged compositions is still time-consuming. We propose a method for designing a series of compositions with simultaneous band convergence in the high-entropy YbxCa1-xMgyZn2-ySb2 material by zeroing the weighted sum of crystal-field splitting energies of the parent compounds. We found that so-designed compositions have both larger power factors and lower thermal conductivities and that one of these compositions exhibits a large thermoelectric figure of merit value in comparison with to other p-type Zintls. Our material shows high stability both thermally and temporally. We then assembled an all-Zintl single-stage module, nontoxic and free of tellurium, that demonstrates an exceptional heat-to-electricity conversion efficiency exceeding 10% at a temperature difference of 475 kelvin.

Precise Fabrication and Manipulation of Individual Polymer Nanofibers.

Polymer nanofibers hold promise in a wide range of applications owing to their diverse properties, flexibility, and cost effectiveness. In this study, we introduce a polymer nanofiber drawing process in a scanning electron microscope and focused ion beam (SEM/FIB) instrument with in situ observation. We employed a nanometer-sharp tungsten needle and prepolymer microcapsules to enable nanofiber drawing in a vacuum environment. This method produces individual polymer nanofibers with diameters as small as ∼500 nm and lengths extending to millimeters, yielding nanofibers with an aspect ratio of 2000:1. The attachment to the tungsten manipulator ensures accurate transfer of the polymer nanofiber to diverse substrate types as well as fabrication of assembled structures. Our findings provide valuable insights into ultrafine polymer fiber drawing, paving the way for high-precision manipulation and assembly of polymer nanofibers.

Multifunctional Applications Enabled by Fluorination of Hexagonal Boron Nitride.

2D materials exhibit exceptional properties as compared to their macroscopic counterparts, with promising applications in nearly every area of science and technology. To unlock further functionality, the chemical functionalization of 2D structures is a powerful technique that enables tunability and new properties within these materials. Here, the successful effort to chemically functionalize hexagonal boron nitride (hBN), a chemically inert 2D ceramic with weak interlayer forces, using a gas-phase fluorination process is exploited. The fluorine functionalization guides interlayer expansion and increased polar surface charges on the hBN sheets resulting in a number of vastly improved applications. Specifically, the F-hBN exhibits enhanced dispersibility and thermal conductivity at higher temperatures by more than 75% offering exceptional performance as a thermofluid additive. Dispersion of low volumes of F-hBN in lubricating oils also offers marked improvements in lubrication and wear resistance for steel tribological contacts decreasing friction by 31% and wear by 71%. Additionally, incorporating numerous negatively charged fluorine atoms on hBN induces a permanent dipole moment, demonstrating its applicability in microelectronic device applications. The findings suggest that anchoring chemical functionalities to hBN moieties improves a variety of properties for h-BN, making it suitable for numerous other applications such as fillers or reinforcement agents and developing high-performance composite structures.

Effect of Alkyl Chain Length on the Corrosion Inhibition Performance of Imidazolium-Based Ionic Liquids for Carbon Steel in 1 M HCl Solution: Experimental Evaluation and Theoretical Analysis.

In this study, five kinds of 1-alkyl-3-methylimidazolium bromide ([CXami]Br) ionic liquids with different alkyl chain lengths (8, 10, 12, 14, and 16) were selected as inhibitors. Then, their corrosion inhibition performances for Q235 steel in 1.0 mol L-1 HCl solution were investigated via a weight loss test, polarization curve method, and surface analysis techniques. The results show that these five imidazolium-based ionic liquids are all mixed-type inhibitors, and they can be spontaneously adsorbed onto the Q235 steel surface. The adsorption process follows the Langmuir model and involves mixed physical-chemical adsorption. Theoretical calculations confirm that the increase in alkyl chain length is conducive to the imidazolium-based ionic liquids exhibiting stronger chemical bonding abilities and forming denser adsorption films. The inhibition efficiency significantly increases below the critical micelle concentration (CMC) with an increase in alkyl chain length, and the highest inhibition efficiency is 95.17% for the [C16ami]Br inhibitor at the concentration of 0.005 mM. However, above the CMC, the inhibition efficiency is minimally affected by the alkyl chain length since all ionic liquid inhibitors have reached adsorption saturation on the steel surface.

Tuning Local Atomic Structures in MoS2 Based Catalysts for Electrochemical Nitrate Reduction.

In recent years, there has been a substantial surge in the investigation of transition-metal dichalcogenides such as MoS2 as a promising electrochemical catalyst. Inspired by denitrification enzymes such as nitrate reductase and nitrite reductase, the electrochemical nitrate reduction catalyzed by MoS2 with varying local atomic structures is reported. It is demonstrated that the hydrothermally synthesized MoS2 containing sulfur vacancies behaves as promising catalysts for electrochemical denitrification. With copper doping at less than 9% atomic ratio, the selectivity of denitrification to dinitrogen in the products can be effectively improved. X-ray absorption characterizations suggest that two sulfur vacancies are associated with one copper dopant in the MoS2 skeleton. DFT calculation confirms that copper dopants replace three adjacent Mo atoms to form a trigonal defect-enriched region, introducing an exposed Mo reaction center that coordinates with Cu atom to increase N2 selectivity. Apart from the higher activity and selectivity, the Cu-doped MoS2 also demonstrates remarkably improved tolerance toward oxygen poisoning at high oxygen concentration. Finally, Cu-doped MoS2 based catalysts exhibit very low specific energy consumption during the electrochemical denitrification process, paving the way for potential scale-up operations.

Low-temperature grapho-epitaxial La-substituted BiFeO3 on metallic perovskite.

Bismuth ferrite has garnered considerable attention as a promising candidate for magnetoelectric spin-orbit coupled logic-in-memory. As model systems, epitaxial BiFeO3 thin films have typically been deposited at relatively high temperatures (650-800 °C), higher than allowed for direct integration with silicon-CMOS platforms. Here, we circumvent this problem by growing lanthanum-substituted BiFeO3 at 450 °C (which is reasonably compatible with silicon-CMOS integration) on epitaxial BaPb0.75Bi0.25O3 electrodes. Notwithstanding the large lattice mismatch between the La-BiFeO3, BaPb0.75Bi0.25O3, and SrTiO3 (001) substrates, all the layers in the heterostructures are well ordered with a [001] texture. Polarization mapping using atomic resolution STEM imaging and vector mapping established the short-range polarization ordering in the low temperature grown La-BiFeO3. Current-voltage, pulsed-switching, fatigue, and retention measurements follow the characteristic behavior of high-temperature grown La-BiFeO3, where SrRuO3 typically serves as the metallic electrode. These results provide a possible route for realizing epitaxial multiferroics on complex-oxide buffer layers at low temperatures and opens the door for potential silicon-CMOS integration.

Regulating Anionic Redox via Mg Substitution in Mn-Rich Layered Oxide Cathodes Enabling High Electrochemical Stability for Sodium-Ion Batteries.

With the limited resources and high cost of lithium-ion batteries (LIBs) and the ever-increasing market demands, sodium-ion batteries (SIBs) gain much interest due to their economical sustainability, and similar chemistry and manufacturing processes to LIBs. As cathodes play a vital role in determining the energy density of SIBs, Mn-based layered oxides are promising cathodes due to their low cost, environmental friendliness, and high theoretical capacity. However, the main challenge is structural instability upon cycling at high voltage. Herein, Mg is introduced into the P2-type Na0.62 Ni0.25 Mn0.75 O2 cathode to enhance electrochemical stability. By combining electrochemical testing and material characterizations, it is found that substituting 10 mol% Mg can effectively alleviate the P2-O2 phase transition, Jahn-Teller distortion, and irreversible oxygen redox. Moreover, structural integrity is greatly improved. These lead to enhanced electrochemical performances. With the optimized sample, a remarkable capacity retention of 92% in the half cell after 100 cycles and 95% in the full cell after 170 cycles can be achieved. Altogether, this work provides an alternative way to stabilize P2-type Mn-based layer oxide cathodes, which in turn, put forward the development of this material for the next-generation SIBs.

Cooperative Copper Single-Atom Catalyst in 2D Carbon Nitride for Enhanced CO2 Electrolysis to Methane.

Renewable-electricity-powered carbon dioxide (CO2) reduction (eCO2R) to high-value fuels like methane (CH4) holds the potential to close the carbon cycle at meaningful scales. However, this kinetically staggered 8-electron multistep reduction suffers from inadequate catalytic efficiency and current density. Atomic Cu-structures can boost eCO2R-to-CH4 selectivity due to enhanced intermediate binding energies (BEs) resulting from favorably shifted d-band centers. In this work, 2D carbon nitride (CN) matrices, viz. Na-polyheptazine (PHI) and Li-polytriazine imides (PTI), are exploited to host Cu-N2 type single-atom sites with high density (≈1.5 at%), via a facile metal-ion exchange process. Optimized Cu loading in nanocrystalline Cu-PTI maximizes eCO2R-to-CH4 performance with Faradaic efficiency (FECH4) of ≈68% and a high partial current density of 348 mA cm-2 at -0.84 V vs reversible hydrogen electrode (RHE), surpassing the state-of-the-art catalysts. Multi-Cu substituted N-appended nanopores in the CN frameworks yield thermodynamically stable quasi-dual/triple sites with large interatomic distances dictated by the pore dimensions. First-principles calculations elucidate the relative Cu-CN cooperative effects between the matrices and how the Cu local environment dictates the adsorbate BEs, density of states, and CO2-to-CH4 energy profile landscape. The 9N pores in Cu-PTI yield cooperative Cu-Cu sites that synergistically enhance the kinetics of the rate-limiting steps in the eCO2R-to-CH4 pathway.

Enhanced photo-Fenton degradation of contaminants in a wide pH range via synergistic interaction between 1T and 2H MoS2 and copolymer tea polyphenols/polypyrrole.

In this study, we present the successful development of a unique photo-Fenton catalyst, 1T-2H MoS2@TP/PPy (MTP), achieved through the coating of a copolymer of tea polyphenol (TP) and polypyrrole (PPy) onto the surface of heterophase molybdenum disulfide (1T-2H MoS2). This innovative approach involves the integration of hydrothermal synthesis with copolymerization techniques. Our strategy utilizes nanoflower-like 1T-2H MoS2 as the foundational framework, which is then enveloped in TP and PPy copolymer. This innovative approach involves the integration of hydrothermal synthesis with copolymerization techniques. Our strategy utilizes nanoflower-like 1T-2H MoS2 as the foundational framework, which is then enveloped in TP and PPy copolymer. This distinctive architecture demonstrates exceptional catalytic performance owing to the hetero-phase entanglement of 1T-2H MoS2, which provides a diverse array of active sites. The coupled structure of TP and iron (TP-Fe2+/Fe3+) effectively overcome the limitation associated with the iron source. The incorporation of PPy not only reduces the recombination of photogenerated electron-hole pairs but also enhances the stability of 1T-2H MoS2. Remarkably, our experiments on the degradation of methylene blue (MB) and tetracycline (TC) degradation demonstrate that TP-Fe2+/Fe3+ significantly expands the pH applicability range of the MTP composite catalyst. Additionally, we examine several factors, including different catalysts, H2O2 addition, variations in light intensity, solution pH, temperature fluctuations, and the role of active species, to comprehensively understand their impact on the photo-Fenton degradation process. In conclusion, MTP composite exhibits robust catalytic stability and demonstrates a broad pH utilization range in the photo-Fenton oxidation process, highlighting its promising potential for a wide range of applications.

Cascaded compression of size distribution of nanopores in monolayer graphene.

Monolayer graphene with nanometre-scale pores, atomically thin thickness and remarkable mechanical properties provides wide-ranging opportunities for applications in ion and molecular separations1, energy storage2 and electronics3. Because the performance of these applications relies heavily on the size of the nanopores, it is desirable to design and engineer with precision a suitable nanopore size with narrow size distributions. However, conventional top-down processes often yield log-normal distributions with long tails, particularly at the sub-nanometre scale4. Moreover, the size distribution and density of the nanopores are often intrinsically intercorrelated, leading to a trade-off between the two that substantially limits their applications5-9. Here we report a cascaded compression approach to narrowing the size distribution of nanopores with left skewness and ultrasmall tail deviation, while keeping the density of nanopores increasing at each compression cycle. The formation of nanopores is split into many small steps, in each of which the size distribution of all the existing nanopores is compressed by a combination of shrinkage and expansion and, at the same time as expansion, a new batch of nanopores is created, leading to increased nanopore density by each cycle. As a result, high-density nanopores in monolayer graphene with a left-skewed, short-tail size distribution are obtained that show ultrafast and ångström-size-tunable selective transport of ions and molecules, breaking the limitation of the conventional log-normal size distribution9,10. This method allows for independent control of several metrics of the generated nanopores, including the density, mean diameter, standard deviation and skewness of the size distribution, which will lead to the next leap in nanotechnology.

An Investigation of PPy@1T/2H MoS2 Composites with Durable Photothermal-Promoted Effect in Photo-Fenton Degradation of Methylene Blue and in Water Evaporation.

MoS2 has garnered considerable attention as an exceptional co-catalyst that is capable of significantly enhancing the efficiency of H2O2 decomposition in advanced oxidation processes (AOPs). This improvement allows for a reduction in the required amounts of H2O2 and Fe2+. In this study, we investigated the cyclic durability of photo-Fenton catalysts, focusing on the degradation of pollutants through the introduction of PPy into heterogeneous 1T-2H MoS2 units. The resulting photothermal-Fenton catalysts, comprising non-ferrous Fenton catalysts, demonstrated excellent degradation performance for simulated pollutants. In comparison with 1T-2H MoS2, the PPy@1T-2H MoS2 composite exhibited remarkable stability and photothermal enhancement in the photo-Fenton degradation of methylene blue (MB) under visible light irradiation. The photo-Fenton reaction efficiently degraded contaminants, achieving 99% removal within 5 min and 99.8% removal within 30 min. Moreover, the co-catalyst complex displayed enhanced cyclic stability during the photo-Fenton reaction, with a contaminant removal efficiency of 92%, even after the 13th cyclic test. The combined effects of PPy and 1T-2H MoS2 demonstrated improved efficiency in both photocatalytic and photo-Fenton catalytic reactions. Furthermore, PPy@1T-2H MoS2 exhibited outstanding performance in the photothermal evaporation of water, achieving an efficiency of 86.3% under one solar irradiation.

Solutions Are the Problem: Ordered Two-Dimensional Covalent Organic Framework Films by Chemical Vapor Deposition.

Covalent organic frameworks (COFs) are a promising class of crystalline polymer networks that are useful due to their high porosity, versatile functionality, and tunable architecture. Conventional solution-based methods of producing COFs are marred by slow reactions that produce powders that are difficult to process into adaptable form factors for functional applications, and there is a need for facile and fast synthesis techniques for making crystalline and ordered covalent organic framework (COF) thin films. In this work, we report a chemical vapor deposition (CVD) approach utilizing co-evaporation of two monomers onto a heated substrate to produce highly crystalline, defect-free COF films and coatings with hydrazone, imine, and ketoenamine COF linkages. This all-in-one synthesis technique produces highly crystalline, 40 nm-1 µm-thick COF films on Si/SiO2 substrates in less than 30 min. Crystallinity and alignment were proven by using a combination of grazing-incidence wide-angle X-ray scattering (GIWAXS) and transmission electron microscopy (TEM), and successful conversion of the monomers to produce the target COF was supported by Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and UV-vis measurements. Additionally, we used atomic force microscopy (AFM) to investigate the growth mechanisms of these films, showing the coalescence of triangular crystallites into a smooth film. To show the wide applicability and scope of the CVD process, we also prepared crystalline ordered COF films with imine and ketoenamine linkages. These films show potential as high-quality size exclusion membranes, catalytic platforms, and organic transistors.

Battery metal recycling by flash Joule heating.

The staggering accumulation of end-of-life lithium-ion batteries (LIBs) and the growing scarcity of battery metal sources have triggered an urgent call for an effective recycling strategy. However, it is challenging to reclaim these metals with both high efficiency and low environmental footprint. We use here a pulsed dc flash Joule heating (FJH) strategy that heats the black mass, the combined anode and cathode, to >2100 kelvin within seconds, leading to ~1000-fold increase in subsequent leaching kinetics. There are high recovery yields of all the battery metals, regardless of their chemistries, using even diluted acids like 0.01 M HCl, thereby lessening the secondary waste stream. The ultrafast high temperature achieves thermal decomposition of the passivated solid electrolyte interphase and valence state reduction of the hard-to-dissolve metal compounds while mitigating diffusional loss of volatile metals. Life cycle analysis versus present recycling methods shows that FJH significantly reduces the environmental footprint of spent LIB processing while turning it into an economically attractive process.

Vacancy-mediated anomalous phononic and electronic transport in defective half-Heusler ZrNiBi.

Studies of vacancy-mediated anomalous transport properties have flourished in diverse fields since these properties endow solid materials with fascinating photoelectric, ferroelectric, and spin-electric behaviors. Although phononic and electronic transport underpin the physical origin of thermoelectrics, vacancy has only played a stereotyped role as a scattering center. Here we reveal the multifunctionality of vacancy in tailoring the transport properties of an emerging thermoelectric material, defective n-type ZrNiBi. The phonon kinetic process is mediated in both propagating velocity and relaxation time: vacancy-induced local soft bonds lower the phonon velocity while acoustic-optical phonon coupling, anisotropic vibrations, and point-defect scattering induced by vacancy shorten the relaxation time. Consequently, defective ZrNiBi exhibits the lowest lattice thermal conductivity among the half-Heusler family. In addition, a vacancy-induced flat band features prominently in its electronic band structure, which is not only desirable for electron-sufficient thermoelectric materials but also interesting for driving other novel physical phenomena. Finally, better thermoelectric performance is established in a ZrNiBi-based compound. Our findings not only demonstrate a promising thermoelectric material but also promote the fascinating vacancy-mediated anomalous transport properties for multidisciplinary explorations.

Boosting Oxygen Evolution Reaction of (Fe,Ni)OOH via Defect Engineering for Anion Exchange Membrane Water Electrolysis Under Industrial Conditions.

Developing non-precious catalysts with long-term catalytic durability and structural stability under industrial conditions is the key to practical alkaline anion exchange membrane (AEM) water electrolysis. Here, an energy-saving approach is proposed to synthesize defect-rich iron nickel oxyhydroxide for stability and efficiency toward the oxygen evolution reaction. Benefiting from in situ cation exchange, the nanosheet-nanoflake-structured catalyst is homogeneously embedded in, and tightly bonded to, its substrate, making it ultrastable at high current densities. Experimental and theoretical calculation results reveal that the introduction of Ni in FeOOH reduces the activation energy barrier for the catalytic reaction and that the purposely created oxygen defects not only ensure the exposure of active sites and maximize the effective catalyst surface but also modulate the local coordination environment and chemisorption properties of both Fe and Ni sites, thus lowering the energy barrier from *O to *OOH. Consequently, the optimized d-(Fe,Ni)OOH catalyst exhibits outstanding catalytic activity with long-term durability under both laboratory and industrial conditions. The large-area d-(Fe,Ni)OOH||NiMoN pair requires 1.795 V to reach a current density of 500 mA cm-2 at an absolute current of 12.5 A in an AEM electrolyzer for overall water electrolysis, showing great potential for industrial water electrolysis.

Three-dimensional covalent organic frameworks with pto and mhq-z topologies based on Tri- and tetratopic linkers.

Three-dimensional (3D) covalent organic frameworks (COFs) possess higher surface areas, more abundant pore channels, and lower density compared to their two-dimensional counterparts which makes the development of 3D COFs interesting from a fundamental and practical point of view. However, the construction of highly crystalline 3D COF remains challenging. At the same time, the choice of topologies in 3D COFs is limited by the crystallization problem, the lack of availability of suitable building blocks with appropriate reactivity and symmetries, and the difficulties in crystalline structure determination. Herein, we report two highly crystalline 3D COFs with pto and mhq-z topologies designed by rationally selecting rectangular-planar and trigonal-planar building blocks with appropriate conformational strains. The pto 3D COFs show a large pore size of 46 Å with an extremely low calculated density. The mhq-z net topology is solely constructed from totally face-enclosed organic polyhedra displaying a precise uniform micropore size of 1.0 nm. The 3D COFs show a high CO2 adsorption capacity at room temperature and can potentially serve as promising carbon capture adsorbents. This work expands the choice of accessible 3D COF topologies, enriching the structural versatility of COFs.

Superior mechanical properties of multilayer covalent-organic frameworks enabled by rationally tuning molecular interlayer interactions.

Two-dimensional (2D) covalent-organic frameworks (COFs) with a well-defined and tunable periodic porous skeleton are emerging candidates for lightweight and strong 2D polymeric materials. It remains challenging, however, to retain the superior mechanical properties of monolayer COFs in a multilayer stack. Here, we successfully demonstrated a precise layer control in synthesizing atomically thin COFs, enabling a systematic study of layer-dependent mechanical properties of 2D COFs with two different interlayer interactions. It was shown that the methoxy groups in COFTAPB-DMTP provided enhanced interlayer interactions, leading to layer-independent mechanical properties. In sharp contrast, mechanical properties of COFTAPB-PDA decreased significantly as the layer number increased. We attributed these results to higher energy barriers against interlayer sliding due to the presence of interlayer hydrogen bonds and possible mechanical interlocking in COFTAPB-DMTP, as revealed by density functional theory calculations.

Fluorinated Multi-Walled Carbon Nanotubes Coated Separator Mitigates Polysulfide Shuttle in Lithium-Sulfur Batteries.

Li-S batteries still suffer from two of the major challenges: polysulfide shuttle and low inherent conductivity of sulfur. Here, we report a facile way to develop a bifunctional separator coated with fluorinated multiwalled carbon nanotubes. Mild fluorination does not affect the inherent graphitic structure of carbon nanotubes as shown by transmission electron microscopy. Fluorinated carbon nanotubes show an improved capacity retention by trapping/repelling lithium polysulfides at the cathode, while simultaneously acting as the "second current collector". Moreover, reduced charge-transfer resistance and enhanced electrochemical performance at the cathode-separator interface result in a high gravimetric capacity of around 670 mAh g-1 at 4C. Unique chemical interactions between fluorine and carbon at the separator and the polysulfides, studied using DFT calculations, establish a new direction of utilizing highly electronegative fluorine moieties and absorption-based porous carbons for mitigation of polysulfide shuttle in Li-S batteries.

Branching phenomena in nanostructure synthesis illuminated by the study of Ni-based nanocomposites.

Branching phenomena are ubiquitous in both natural and artificial crystallization processes. The branched nanostructures' emergent properties depend upon their structures, but their structural tunability is limited by an inadequate understanding of their formation mechanisms. Here we developed an ensemble of Nickel-Based nano-Composites (NBCs) to investigate branching phenomena in solution-phase synthesis with precision and in depth. NBCs of 24 morphologies, including dots, core@shell dots, hollow shells, clusters, polyhedra, platelets, dendrites, urchins, and dandelions, were synthesized through systematic adjustment of multiple synthesis parameters. Relationships between the synthesis parameters and the resultant morphologies were analyzed. Classical or non-classical models of nucleation, nascent growth, 1D growth, 2D growth, 3D reconstruction, aggregation, and carburization were defined individually and then integrated to provide a holistic view of the formation mechanism of branched NBCs. Finally, guidelines were extracted and verified to guide the rational solution-phase syntheses of branched nanomaterials with emergent biological, chemical, and physical properties for potential applications in immunology, catalysis, energy storage, and optics. Demonstrating a systematic approach for deconvoluting the formation mechanism and enhancing the synthesis tunability, this work is intended to benefit the conception, development, and improvement of analogous artificial branched nanostructures. Moreover, the progress on this front of synthesis science would, hopefully, deepen our understanding of branching phenomena in nature.

Self-Promoting Energy Storage in Balsa Wood-Converted Porous Carbon Coupled with Carbon Nanotubes.

For most electrodes fabricated with carbon, transition metal compounds, or conductive polymers, the capacitance may deteriorate with cyclic charging and discharging. Thus, an electrochemically stable supercapacitor has long been pursued by researchers. In this work, the hierarchical structure of balsa wood is preserved in the converted carbon which is used as a supporting framework to fabricate electrodes for supercapacitors. Well-grown carbon nanotubes (CNTs) on interior and exterior surfaces of balsa carbon channels provide two advantages including 1) offering more specific surface area to boost capacitance via electric double layer capacitance and 2) offering more active Fe and Ni sites to participate in the redox reaction to enhance capacitance of the balsa carbon/CNTs electrode. The balsa carbon/CNTs demonstrate an excellent area capacitance of 1940 mF cm-2 . As active sites on Ni and Fe catalysts and inner walls of CNTs are gradually released, the capacitance increases 66% after 4000 charge-discharge cycles. This work brings forward a strategy for the rational design of high-performance biomass carbon coupled with advanced nanostructures for energy storage.