Oxygenate-induced structural evolution of high-entropy electrocatalysts for multifunctional alcohol electrooxidation integrated with hydrogen production.

High-entropy compounds have been emerging as promising candidates for electrolysis, yet their controllable electrosynthesis strategy remains a formidable challenge because of the ambiguous ionic interaction and codeposition mechanism. Herein, we report a oxygenates directionally induced electrodeposition strategy to construct high-entropy materials with amorphous features, on which the structural evolution from high-entropy phosphide to oxide is confirmed by introducing vanadate, thus realizing the simultaneous optimization of composition and structure. The representative P-CoNiMnWVOx shows excellent bifunctional catalytic performance toward alkaline hydrogen evolution reaction and ethanol oxidation reaction (EOR), with small potentials of -168 mV and 1.38 V at 100 mA cm-2, respectively. In situ spectroscopy illustrates that the electrochemical reconstruction of P-CoNiMnWVOx induces abundant Co-O species as the main catalytic active species for EOR and follows the conversion pathway of the C2 product. Theoretical calculations reveal the optimized electronic structure and adsorption free energy of reaction intermediates on P-CoNiMnWVOx, thereby resulting in a facilitated kinetic process. A membrane-free electrolyzer delivers both high Faradaic efficiencies of acetate and H2 over 95% and superior stability at100 mA cm-2 during 120 h electrolysis. In addition, the unique composition and structural advantages endow P-CoNiMnWVOx with multifunctional catalytic activity and realize multipathway electrosynthesis of formate-coupled hydrogen production.

Structural and Evolutionary Analysis of Proteins Endowed with a Nucleotidyltransferase, or Non-canonical Palm, Catalytic Domain.

Many polymerases and other proteins are endowed with a catalytic domain belonging to the nucleotidyltransferase fold, which has also been deemed the non-canonical palm domain, in which three conserved acidic residues coordinate two divalent metal ions. Tertiary structure-based evolutionary analyses provide valuable information when the phylogenetic signal contained in the primary structure is blurry or has been lost, as is the case with these proteins. Pairwise structural comparisons of proteins with a nucleotidyltransferase fold were performed in the PDBefold web server: the RMSD, the number of superimposed residues, and the Qscore were obtained. The structural alignment score (RMSD × 100/number of superimposed residues) and the 1-Qscore were calculated, and distance matrices were constructed, from which a dendogram and a phylogenetic network were drawn for each score. The dendograms and the phylogenetic networks display well-defined clades, reflecting high levels of structural conservation within each clade, not mirrored by primary sequence. The conserved structural core between all these proteins consists of the catalytic nucleotidyltransferase fold, which is surrounded by different functional domains. Hence, many of the clades include proteins that bind different substrates or partake in non-related functions. Enzymes endowed with a nucleotidyltransferase fold are present in all domains of life, and participate in essential cellular and viral functions, which suggests that this domain is very ancient. Despite the loss of evolutionary traces in their primary structure, tertiary structure-based analyses allow us to delve into the evolution and functional diversification of the NT fold.

Discovery of a series of silicon-based ferrimagnets in CrMnSin (n = 4-20) clusters.

Herein, the structural evolution, electronic and magnetic properties of silicon clusters with two different dopants, CrMnSin (n = 4-20) clusters were investigated at density functional theory (DFT) level. Small-sized CrMnSin (n = 4-9) clusters tend to adopt bipyramid-based geometries, while clusters with sizes n = 10 and 11 prefer to opening cage-like structures. For sizes n = 12 to 14, the half-encapsulated structures gradually transform into closed-cage Cr@Sin structures, with the Mn atom exposed outside. Starting from size 15, both the Cr and Mn atoms are completely encapsulated by silicon atoms. Meanwhile, the Cr and Mn atoms in smaller-sized CrMnSin (n = 4-7) clusters tend to be separated, while they prefer to stay together for larger sizes. Cr atom always acts as electron donor, but not for Mn atom. From the average binding energies, one can conclude that it is easier to form larger size clusters. Smaller and larger sized CrMnSin (n = 4-9 and 19-20) clusters prefer to exhibit ferromagnetic Cr-Mn coupling, while sizes n = 10-18 always exhibit ferrimagnetic state. To our knowledge, the CrMnSin clusters is the first kind of neutral transition-metal doped semiconductor clusters that show ferrimagnetic state within a wide size range.

Magnetic properties of CrMnGen (n = 3-20) clusters.

Due to the potential applications in next-generation micro/nano electronic devices and functional materials, magnetic germanium (Ge)-based clusters are receiving increasing attention. In this work, we reported the structures, electronic and magnetic properties of CrMnGen with sizes n = 3-20. Transition metals (TMs) of Cr and Mn tend to stay together and be surrounded by Ge atoms. Small sized clusters with n ≤ 8 prefer to adopt bipyramid-based structures as the motifs with the excess Ge atoms absorbed on the surface. Starting from n = 9, the structure with one TM atom interior appears and persists until n = 16, and for larger sizes n = 17-20, the two TM atoms are full-encapsulated by Ge atoms to form endohedral structures. The Hirshfeld population analyses show that Cr atom always acts as the electron donor, while Mn atom is always the acceptor except for sizes 3 and 6. The average binding energies of these clusters increase with cluster size n, sharing a very similar trend as that of CrMnSin (n = 4-20) clusters, which indicates that it is favorable to form large-sized clusters. CrMnGen (n = 6, 13, 16, 19, and 20) clusters prefer to exhibit ferromagnetic Cr-Mn coupling, while the remaining clusters are ferrimagnetic.

Unraveling the Potential Dependence of Active Structures and Reaction Mechanism of Ni-based MOFs Electrocatalysts for Alkaline OER.

Nickel-based metal-organic frameworks (MOFs) with flexible structure units provide a broad platform for designing highly efficient electrocatalysts, especially for alkaline oxygen evolution reaction (OER). However, the stability of MOFs under harsh and dynamic reaction conditions poses significant challenges, resulting in ambiguous structure-activity relationships in MOFs-based OER research. Herein, Ni-benzenedicarboxylic acid-based MOF (NiBDC) is selected as prototypical catalyst to elucidate  its real active sites for OER and reaction pathway under different reaction states. Electrochemical measurements combined with X-ray absorption spectroscopy (XAS) and Raman spectroscopy reveal that the complete reconstruction of NiBDC to ß-NiOOH in the chronoamperometry activation process is responsible for significantly increased OER performance. In situ XAS and Raman results further demonstrate the electro-oxidation of ß-NiOOH into γ-NiOOH at high-potential state (above 1.6 V vs RHE). Furthermore, the collective evidences from key reaction intermediates and isotope-labeled products definitely unravel the potential dependence of OER mechanism: OER process at low-potential state proceeds mainly through the lattice oxygen-mediated mechanism, while adsorbate evolution mechanism emerges as the predominant pathway at high-potential state. Interestingly, the dynamically changing OER mechanism can not only reduce the required overpotential at the low-potential state but also improve the electrochemical stability of catalysts at high-potential state.

14-Electron Redox Chemistry Enabled by Salen-Based π-Conjugated Framework Polymer Boosting High-Performance Lithium-Ion Storage.

A paucity of redox centers, poor charge transport properties, and low structural stability of organic materials obstruct their use in practical applications. Herein, these issues have been addressed through the use of a redox-active salen-based framework polymer (RSFP) containing multiple redox-active centers in π-conjugated configuration for applications in lithium-ion batteries (LIBs). Based on its unique architecture, RSFP exhibits a superior reversible capacity of 671.8 mAh g-1 at 0.05 A g-1 after 168 charge-discharge cycles. Importantly, the lithiation/de-lithiation performance is enhanced during operation, leading to an unprecedented reversible capacity of 946.2 mAh g-1 after 3500 cycles at 2 A g-1. The structural evolution of RSFP is studied ex situ using X-ray photoelectron spectroscopy, revealing multiple active C═N, C─O, and C═O sites and aromatic sites such as benzene rings. Remarkably, the emergence of C═O originated from C─O is triggered by an electrochemical process, which is beneficial for improving reversible lithiation/delithiation behavior. Furthermore, the respective strong and weak binding interactions between redox centers and lithium ions, corresponding to theoretical capacities of 670.1 and 938.2 mAh g-1, have been identified by density functional theory calculations manifesting 14-electron redox reactions. This work sheds new light on routes for the development of redox-active organic materials for energy storage applications.

Structural Evolution of Manganese Prussian Blue Analogue in Aqueous ZnSO4 Electrolyte.

Among different Prussian Blue Analogues (PBAs), manganese hexacyanoferrate (MnHCF), with open framework and two abundant electroactive metal sites, exhibits high potential for the grid-scale aqueous rechargeable zinc-ion batteries (ARZIBs) application. Until now, the intercalation mechanism of Zn2+ into MnHCF has not been clearly illustrated. In this work, combining different synchrotron X-ray techniques, the structural and microscopic evolution of MnHCF in 3 m ZnSO4 electrolyte is comprehensively studied, and a thorough understanding of the intercalation/release dynamic, in terms of local and long-range domain, is provided. The elemental distribution and structural information of Fe, Mn, Zn inside MnHCF electrodes is obtained from the X-ray fluorescence (XRF) elemental maps and X-ray absorption spectroscopy (XAS). The in-depth analysis of extended X-ray absorption fine structure (EXAFS) signals confirm that the rearrangement of Mn site, evidencing the cleavage of the Mn─N bond with the formation of a Mn─O bond, in an octahedral environment. The phase transformation of MnHCF takes place exclusively during the 1st cycle, and a mixture of rhombohedral and cubic zinc hexacynoferrate (ZnHCF) phases are formed during the first charge process. Thereafter, the newly formed cubic ZnHCF phase becomes the only stable one, existing in the subsequent cycles and exhibiting excellent electrochemical stability.

Selective Lattice Doping Enables a Low-Cost, High-Capacity and Long-Lasting Potassium Layered Oxide Cathode for Potassium and Sodium Storage.

Layered transition metal oxides are highly promising host materials for K ions, owing to their high theoretical capacities and appropriate operational potentials. To address the intrinsic issues of KxMnO2 cathodes and optimize their electrochemical properties, a novel P3-type oxide doped with carefully chosen cost-effective, electrochemically active and multi-functional elements is proposed, namely K0.57Cu0.1Fe0.1Mn0.8O2. Compared to the pristine K0.56MnO2, its reversible specific is increased from 104 to 135 mAh g-1. In addition, the Cu and Fe co-doping triples the capacity under high current densities, and contributes to long-term stability over 500 cycles with a capacity retention of 68 %. Such endeavor holds the potential to make potassium-ion batteries particularly competitive for application in sustainable, low-cost, and large-scale energy storage devices. In addition, the cathode is also extended for sodium storage. Facilitated by the interlayer K ions that protect the layered structure from collapsing and expand the diffusion pathway for sodium ions, the cathode shows a high reversible capacity of 144 mAh g-1, fast kinetics and a long lifespan over 1000 cycles. The findings offer a novel pathway for the development of high-performance and cost-effective sodium-ion batteries.

Determination of Ground State Structures of Snx - (x=21-35) Clusters.

In this work, an unbiased global search with a homemade genetic algorithm was performed to investigate the structural evolution and electronic properties of Snx - (x=21-35) clusters with density functional theory (DFT) calculations. All the ground-state structures for all these Snx - (x=21-35) clusters have been confirmed by the comparison of the experimental and simulated photoelectron spectra (PESs). It has been revealed that all Snx - (x=21-35) clusters are tricapped trigonal prism (TTP)-based structures consisting of two (for sizes x=21-28) or three (for x=29-35) TTP units, with the remaining atoms adsorbed on the surface or inserted between TTP units. The gradually decreasing HOMO-LUMO gaps indicate that these clusters are undergoing semiconductor-to-metal transformation. The average binding energies show that the structural stabilities of Snx - clusters are not as good as that of silicon and germanium clusters. It found that sizes x=23, 25, 29, 33 show high relative stability.

A ReaxFF Potential for Modeling Organic Matter Degradation with Oxybromine Oxidants.

Oxidation of organic matter with oxybromine oxidants is ushering in a new era of enhanced hydrocarbon recovery. While these potent reagents are being tested in laboratory and field experiments, there is a pressing demand to delineate the molecular processes governing oxidation reactions at geological depth. Here, we parameterize a ReaxFF potential to model the oxidative decompositions of aliphatic and aromatic hydrocarbons in the presence of water-NaBr solutions that contain oxybromine (BrOn)- oxidizers. Our parameterization results in a reliable empirical bond-order potential that accurately calculates bond energies, exhibiting an RMSE of ∼1.18 eV, corresponding to 1.36 % average error. Reproducing bond dissociation and binding energies from Density Functional Theory (DFT), our parameterization proves transferable to aqueous environments. This H/C/O/Na/Br ReaxFF potential accurately reproduces the oxidation pathways of small hydrocarbons with oxybromine oxidizers. This force field captures proton and oxygen transfer, C-C bond tautomerization, and cleavage, leading to ring-opening and chain fragmentation. Molecular dynamic simulations demonstrate the oxidative degradation of aromatic and aliphatic kerogen-like moieties in bulk solutions. We envision that such reactive force fields will be useful to understand better the oxidation reactions of organic matter formed in geological reservoirs for enhanced shale gas recovery and improved carbon dioxide treatments.

Patterning damage mechanisms for two-dimensional crystalline polymers and evaluation for a conjugated imine-based polymer.

High-quality patterning determines the properties of patterned emerging two-dimensional (2D) conjugated polymers and is essential for potential applications in future electronic nanodevices. However, the most suitable patterning method for 2D polymers has yet to be determined because we still do not have a comprehensive understanding of their damage mechanisms by visualizing the structural modification that occurs during the patterning process. Here, the damage mechanisms during patterning of 2D polymers, induced by various patterning methods, are unveiled based on a systematic study of structural damage and edge morphology in an imine-based 2D polymer (polyimine). Patterning using a focused electron beam, focused ion beam (FIB) and mechanical carving is evaluated. The focused electron beam successively introduces a sputtering effect, knock-on displacement damage and massive radiolysis with increasing electron dose from9.46×107electrons nm-2to1.14×1010electrons nm-2. Successful patterning is enabled by knock-on damage but impeded by carbon contamination beyond a critical sample thickness. A FIB creates current-dependent edge morphologies and extensive damage from ion implantation caused by the tail of the unfocused beam. A precisely controlled tip can tear the polyimine film through grain boundaries and hence create a patterning edge with suitable edge roughness for certain application scenarios when beam damage is avoided. Taking structural damage and the resulting quantitative edge roughness into consideration, this study provides a detailed instruction on the proper patterning techniques for 2D crystalline polymers and paves the way for tailored intrinsic properties and device fabrication using these novel materials.

Investigating Temperature-Dependent Microscopic Deformation in Tough and Self-Healing Hydrogel Using Time-Resolved USAXS.

Tough and self-healing hydrogels are typically sensitive to loading rates or temperatures due to the dynamic nature of noncovalent bonds. Understanding the structure evolution under varying loading conditions can provide valuable insights for developing new tough soft materials. In this study, polyampholyte (PA) hydrogel with a hierarchical structure is used as a model system. The evolution of the microscopic structure during loading is investigated under varied loading temperatures. By combining ultra-small angle X-ray scattering (USAXS) and Mooney-Rivlin analysis, it is elucidated that the deformation of bicontinuous hard/soft phase networks is closely correlated with the relaxation dynamics or strength of noncovalent bonds. At high loading temperatures, the gel is soft and ductile, and large affine deformation of the phase-separated networks is observed, correlated with the fast relaxation dynamics of noncovalent bonds. At low loading temperatures, the gel is stiff, and nonaffine deformation occurs from the onset of loading due to the substantial breaking of noncovalent bonds and limited chain mobility as well as weak adaptation of phase deformation to external stretch. This work provides an in-depth understanding of the relationship between structure and performance of tough and self-healing hydrogels.

Understanding the Structural Evolution of IrFeCoNiCu High-Entropy Alloy Nanoparticles under the Acidic Oxygen Evolution Reaction.

High-entropy alloy (HEA) nanoparticles are promising catalyst candidates for the acidic oxygen evolution reaction (OER). Herein, we report the synthesis of IrFeCoNiCu-HEA nanoparticles on a carbon paper substrate via a microwave-assisted shock synthesis method. Under OER conditions in 0.1 M HClO4, the HEA nanoparticles exhibit excellent activity with an overpotential of ∼302 mV measured at 10 mA cm-2 and improved stability over 12 h of operation compared to the monometallic Ir counterpart. Importantly, an active Ir-rich shell layer with nanodomain features was observed to form on the surface of IrFeCoNiCu-HEA nanoparticles immediately after undergoing electrochemical activation, mainly due to the dissolution of the constituent 3d metals. The core of the particles was able to preserve the characteristic homogeneous single-phase HEA structure without significant phase separation or elemental segregation. This work illustrates that under acidic operating conditions, the near-surface structure of HEA nanoparticles is susceptible to a certain degree of structural dynamics.

Nano Fe3O4 improved the electron donating capacity of dissolved organic matter during sludge composting.

The effect of Fe3O4 nanoparticles (Fe3O4 NPs) on the electron transfer process in aerobic composting systems remains unexplored. In this study, we compared the electron transfer characteristics of DOM in sludge composting without additives (group CK) and with the addition of 50 mg/kg Fe3O4 NPs additive (group Fe). It was demonstrated that the electron transfer capacity (ETC) and electron donating capacity (EDC) of compost-derived DOM increased by 13%-29% and 40%-47%, respectively, with the addition of Fe3O4 NPs during sludge composting. Analyzing the composition and structure of DOM revealed that Fe3O4 NPs promoted the formation of humic acid-like substances and enhanced the aromatic condensation degree of DOM. Correlation analysis indicated that the increase in EDC of DOM was closely associated with the phenolic group in DOM and influenced by quinone groups and the degree of aromatization of DOM. The higher EDC and the structural evolution of DOM in group Fe reduced the bioaccessibility of Cu, Cr, Ni, Zn. This study contributes to a deeper understanding of the redox evolutionary mechanism of DOM in sludge composting and broadens the application of iron oxides additives.

Revealing the anti-sintering phenomenon on silica-supported nickel catalysts during CO2 hydrogenation.

The CO2 catalytic hydrogenation represents a promising approach for gas-phase CO2 utilization in a direct manner. Due to its excellent hydrogenation ability, nickel has been widely studied and has shown good activities in CO2 hydrogenation reactions, in addition to its high availability and low price. However, Ni-based catalysts are prone to sintering under elevated temperatures, leading to unstable catalytic performance. In the present study, various characterization techniques were employed to study the structural evolution of Ni/SiO2 during CO2 hydrogenation. An anti-sintering phenomenon is observed for both 9% Ni/SiO2 and 1% Ni/SiO2 during CO2 hydrogenation at 400°C. Results revealed that Ni species were re-dispersed into smaller-sized nanoparticles and formed Ni0 active species. While interestingly, this anti-sintering phenomenon leads to distinct outcomes for two catalysts, with a gradual increase in both reactivity and CH4 selectivity for 9% Ni/SiO2 presumably due to the formation of abundant surface Ni° from redispersion, while an apparent decreasing trend of CH4 selectivity for 1% Ni/SiO2 sample, presumably due to the formation of ultra-small nanoparticles that diffuse and partially filled the mesoporous pores of the silica support over time. Finally, the redispersion phenomenon was found relevant to the H2 gas in the reaction environment and enhanced as the H2 concentration increased. This finding is believed to provide in-depth insights into the structural evolution of Ni-based catalysts and product selectivity control in CO2 hydrogenation reactions.

Correlating Structural Disorder in Metal (Oxy)hydroxides and Catalytic Activity in Electrocatalytic Oxygen Evolution.

Understanding the correlation between the structural evolution of electrocatalysts and their catalytic activity is both essential and challenging. In this study, we investigate this correlation in the context of the oxygen evolution reaction (OER) by examining the influence of structural disorder during and after dynamic structural evolution on the OER activity of Fe-Ni (oxy)hydroxide catalysts using operando X-ray absorption spectroscopy, alongside other experiments and theoretical calculations. The Debye-Waller factors obtained from extended X-ray absorption fine structure analyses reflect the degree of structural disorder and exhibit a robust correlation with the intrinsic OER activities of the electrocatalysts. The enhanced OER activity of in situ-generated metal (oxy)hydroxides derived from different pre-catalysts is linked to increased structural disorder, offering a promising approach for designing efficient OER electrocatalysts. This strategy may inspire similar investigations in related electrocatalytic energy-conversion systems.

Unveiling the Aggregation of M-N-C Single-Atom Electrocatalysts into Highly Efficient MOOH Nanoclusters during Alkaline Water Oxidation.

M-N-C-type single-atom catalysts (SACs) are highly efficient for the electrocatalytic oxygen evolution reaction (OER). And the isolated metal atoms are usually considered real active sites. However, the oxidative structural evolution of coordinated N during the OER will probably damage the structure of M-N-C, hence resulting in a completely different reaction mechanism. Here, we reveal the aggregation of M-N-C materials during the alkaline OER. Taking Ni-N-C as an example, multiple characterizations show that the coordinated N on the surface of Ni-N-C is almost completely dissolved in the form of NO3-, accompanied by the generation of abundant O functional groups on the surface of the carbon support. Accordingly, the Ni-N bonds are broken. Through a dissolution-redeposition mechanism and further oxidation, the isolated Ni atoms are finally converted to NiOOH nanoclusters supported by carbon as the real active sites for the enhanced OER. Fe-N-C and Co-N-C also have similar aggregation mechanism. Our findings provide unique insight into the structural evolution and activity origin of M-N-C-based catalysts under electrooxidative conditions.

Cr2 Gen - (n = 15-20) clusters with two Cr atoms exhibited antiferromagnetic coupling.

In this work, we investigated the structural evolution, electronic and magnetic properties of Cr2 Gen - clusters for n = 15-20 by using density functional theory (DFT) calculations. Low-energy structures for these clusters were fully searched through a self-developed genetic algorithm code combined with DFT calculations. The calculations show that all the two Cr atoms prefer to stay together to form a strong CrCr bond, which-except for size 20-is shorter than the nearest neighbor distance in Cr bulk. Sizes 15 and 16 adopt a wheel-like structure as the structural motif with the extra Ge atoms capped on the top, while larger sizes (n = 17-20) prefer fullerene-like Cr2 @Ge12 motifs. From the results of the average binding energies of Cr2 Gen - , one can conclude that it is easier to form larger size clusters. In these lowest-lying isomers except for size 16, the two Cr atoms contribute opposite magnetic moments for the total magnetic moments of 1 µB , showing an antiferromagnetic state.

Controlled Supramolecular Self-Assembly Pathways by Intramolecular Rotation of D-A Molecular System toward the Signal Differentiation Detection of Toxic Vapors.

Revealing the structural evolution mechanisms of supramolecular self-assembly can facilitate the exploitation of new self-assembly pathways and various functional materials. Here, this work reports a unique intramolecular rotation-induced structural evolution of supramolecular assemblies from a metastable state to a thermodynamically stable state using a twisting D-A molecule. These self-assemblies are applied to the signal differentiation detection of toxic dimethylsulfide (DMS) vapors. The F161 BT monomer of the inactive state is trapped in off-pathway metastable nanospheres, which can disassemble and induce the transformation of the F161 BT monomer into an active state by crossing the energy barrier. Subsequently, the active monomer goes through the processes of nucleation and elongation, forming thermodynamically stable on-pathway microribbons. Adding seeds can accelerate the molecular conformational transformation, generating microribbons with controlled lengths. Opposite fluorescent responses are obtained when exposing the two aggregates to the DMS vapors, allowing the sensitive detection of DMS with enhanced selectivity, which offers tremendous potential in practical applications.

Isostructural Synthesis of Iron-Based Prussian Blue Analogs for Sodium-Ion Batteries.

Rechargeable sodium ion batteries (SIBs) have promising applications in large-scale energy storage systems. Iron-based Prussian blue analogs (PBAs) are considered as potential cathodes owing to their rigid open framework, low-cost, and simple synthesis. However, it is still a challenge to increase the sodium content in the structure of PBAs and thus suppress the generation of defects in the structure. Herein, a series of isostructural PBAs samples are synthesized and the isostructural evolution of PBAs from cubic to monoclinic after modifying the conditions is witnessed. Accompanied by, the increased sodium content and crystallinity are discovered in PBAs structure. The as-obtained sodium iron hexacyanoferrate (Na1.75 Fe[Fe(CN)6 ]0.9743 ·2.76H2 O) exhibits high charge capacity of 150 mAh g-1 at 0.1 C (17 mA g-1 ) and excellent rate performance (74 mAh g-1 at 50 C (8500 mA g-1 )). Moreover, their highly reversible Na+ ions intercalation/de-intercalation mechanism is verified by in situ Raman and Powder X-ray diffraction (PXRD) techniques. More importantly, the Na1.75 Fe[Fe(CN)6 ]0.9743 ·2.76H2 O sample can be directly assembled in a full cell with hard carbon (HC) anode and shows excellent electrochemical performances. Finally, the relationship between PBAs structure and electrochemical performance is summarized and prospected.