Electrochemical biosensor for sensitive detection of SARS-CoV-2 gene fragments using Bi2Se3 topological insulator.

In this study, we have designed an electrochemical biosensor based on topological material Bi2Se3 for the sensitive detection of SARS-CoV-2 in the COVID-19 pandemic. Flake-shaped Bi2Se3 was obtained directly from high-quality single crystals using mechanical exfoliation, and the single-stranded DNA was immobilized onto it. Under optimal conditions, the peak current of the differential pulse voltammetry method exhibited a linear relationship with the logarithm of the concentration of target-complementary-stranded DNA, ranging from 1.0 × 10-15 to 1.0 × 10-11 M, with a detection limit of 3.46 × 10-16 M. The topological material Bi2Se3, with Dirac surface states, enhanced the signal-to-interference plus noise ratio of the electrochemical measurements, thereby improving the sensitivity of the sensor. Furthermore, the electrochemical sensor demonstrated excellent specificity in recognizing RNA. It can detect complementary RNA by amplifying and transcribing the initial DNA template, with an initial DNA template concentration ranging from 1.0 × 10-18 to 1.0 × 10-15 M. Furthermore, the sensor also effectively distinguished negative and positive results by detecting splitting-synthetic SARS-CoV-2 pseudovirus with a concentration of 1 copy/µL input. Our work underscores the immense potential of the electrochemical sensing platform based on the topological material Bi2Se3 in the detection of pathogens during the rapid spread of acute infectious diseases.

Stabilizing the Bulk-Phase and Solid Electrolyte Interphase of Silicon Microparticle Anode by Constructing Gradient-Hierarchically Ordered Conductive Networks.

The poor bulk-phase and interphase stability, attributable to adverse internal stress, impede the cycling performance of silicon microparticles (µSi) anodes and the commercial application for high-energy-density lithium-ion batteries. In this work, a groundbreaking gradient-hierarchically ordered conductive (GHOC) network structure, ingeniously engineered to enhance the stability of both bulk-phase and the solid electrolyte interphase (SEI) configurations of µSi, is proposed. Within the GHOC network architecture, two-dimensional (2D) transition metal carbides (Ti3C2Tx) act as a conductive "brick", establishing a highly conductive inner layer on µSi, while the porous outer layer, composed of one-dimensional (1D) Tempo-oxidized cellulose nanofibers (TCNF) and polyacrylic acid (PAA) macromolecule, functions akin to structural "rebar" and "concrete", effectively preserves the tightly interconnected conductive framework through multiple bonding mechanisms, including covalent and hydrogen bonds. Additionally, Ti3C2Tx enhances the development of a LiF-enriched SEI. Consequently, the µSi-MTCNF-PAA anode presents a high discharge capacity of 1413.7 mAh g-1 even after 500 cycles at 1.0 C. Moreover, a full cell, integrating LiNi0.8Mn0.1Co0.1O2 with µSi-MTCNF-PAA, exhibits a capacity retention rate of 92.0% following 50 cycles. This GHOC network structure can offer an efficacious pathway for stabilizing both the bulk-phase and interphase structure of anode materials with high volumetric strain.

Bipolar Polymeric Protective Layer for Dendrite-Free and Corrosion-Resistant Lithium Metal Anode in Ethylene Carbonate Electrolyte.

The unstable interface between Li metal and ethylene carbonate (EC)-based electrolytes triggers continuous side reactions and uncontrolled dendrite growth, significantly impacting the lifespan of Li metal batteries (LMBs). Herein, a bipolar polymeric protective layer (BPPL) is developed using cyanoethyl (-CH2CH2C≡N) and hydroxyl (-OH) polar groups, aiming to prevent EC-induced corrosion and facilitating rapid, uniform Li+ ion transport. Hydrogen-bonding interactions between -OH and EC facilitates the Li+ desolvation process and effectively traps free EC molecules, thereby eliminating parasitic reactions. Meanwhile, the -CH2CH2C≡N group anchors TFSI- anions through ion-dipole interactions, enhancing Li+ transport and eliminating concentration polarization, ultimately suppressing the growth of Li dendrite. This BPPL enabling Li|Li cell stable cycling over 750 cycles at 10 mA cm-2 for 2 mAh cm-2. The Li|LiNi0.8Mn0.1Co0.1O2 and Li|LiFePO4 full cells display superior electrochemical performance. The BPPL provides a practical strategy to enhanced stability and performance in LMBs application.

Spatially selective defect management of CsPbI3 films for high-performance carbon-based inorganic perovskite solar cells.

Defects formed at the surface, buried interface and grain boundaries (GB) of CsPbI3 perovskite films considerably limit photovoltaic performance. Such defects could be passivated effectively by the most prevalent post modification strategy without compromising the photoelectric properties of perovskite films, but it is still a great challenge to make this strategy comprehensive to different defects spatially distributed throughout the films. Herein, a spatially selective defect management (SSDM) strategy is developed to roundly passivate various defects at different locations within the perovskite film by a facile one-step treatment procedure using a piperazine-1,4-diium tetrafluoroborate (PZD(BF4)2) solution. The small-size PZD2+ cations could penetrate into the film interior and even make it all the way to the buried interface of CsPbI3 perovskite films, while the BF4- anions, with largely different properties from I- anions, mainly anchor on the film surface. Consequently, virtually all the defects at the surface, buried interface and grain boundaries of CsPbI3 perovskite films are effectively healed, leading to significantly improved film quality, enhanced phase stability, optimized energy level alignment and promoted carrier transport. With these films, the fabricated CsPbI3 PSCs based on carbon electrode (C-PSCs) achieve an efficiency of 18.27%, which is among the highest-reported values for inorganic C-PSCs, and stability of 500 h at 85 °C with 65% efficiency maintenance.

Physically and Chemically Stable Molybdenum-Based Composite Electrodes for p-i-n Perovskite Solar Cells.

Metal halide perovskite solar cells (PSCs) have garnered much attention in recent years. Despite the remarkable advancements in PSCs utilizing traditional metal electrodes, challenges such as stability concerns and elevated costs have necessitated the exploration of innovative electrode designs to facilitate industrial commercialization. Herein, a physically and chemically stable molybdenum (Mo) electrode is developed to fundamentally tackle the instability factors introduced by electrodes. The combined spatially resolved element analyses and theoretical study demonstrate the high diffusion barrier of Mo ions within the device. Structural and morphology characterization also reveals the negligible plastic deformation and halide-metal reaction during aging when Mo is in contact with perovskite (PVSK). The electrode/underlayer junction is further stabilized by a thin seed layer of titanium (Ti) to improve Mo film's uniformity and adhesion. Based on a corresponding p-i-n PSCs (ITO/PTAA/PVSK/C60/SnO2/ITO/Ti/Mo), the champion sample could deliver an efficiency of 22.25%, which is among the highest value for PSCs based on Mo electrodes. Meanwhile, the device shows negligible performance decay after 2000 h operation, and retains 91% of the initial value after 1300 h at 50-60 °C. In summary, the multilayer Mo electrode opens an effective avenue to all-round stable electrode design in high-performance PSCs.

Water-Assisted Growth of Twisted 3R-Stacked MoSe2 Spirals and Its Dramatically Enhanced Second Harmonic Generations.

Enhanced second-harmonic generation (SHG) responses are reported in monolayer transition metal dichalcogenides (e.g., MX2 , M: Mo, W; X: S, Se) due to the broken symmetries. The 3R-like stacked MX2 spiral structures possessing the similar broken inversion symmetry should present dramatically enhanced SHG responses, thus providing great flexibility in designing miniaturized on-chip nonlinear optical devices. To achieve this, the first direct synthesis of twisted 3R-stacked chiral molybdenum diselenide (MoSe2 ) spiral structures with specific screw dislocations (SD) arms is reported, via designing a water-assisted chemical vapor transport (CVT) approach. The study also clarifies the formation mechanism of the MoSe2 spiral structures, by precisely regulating the precursor supply accompanying with multiscale characterizations. Significantly, an up to three orders of magnitude enhancement of the SHG responses in twisted 3R stacked MoSe2 spirals is demonstrated, which is proposed to arise from the synergistic effects of broken inversion symmetry, strong light-matter interaction, and band nesting effects. Briefly, the work provides an efficient synthetic route for achieving the 3R-stacked TMDCs spirals, which can serve as perfect platforms for promoting their applications in on-chip nonlinear optical devices.

Engineering Amorphous-Crystallized Interface of ZrNx Barriers for Stable Inverted Perovskite Solar Cells.

It is challenging to achieve long-term stability of perovskite solar cells due to the corrosion and diffusion of metal electrodes. Integration of compact barriers into devices has been recognized as an effective strategy to protect the perovskite absorber and electrode. However, the difficulty is to construct a thin layer of a few nanometers that can delay ion migration and impede chemical reactions simultaneously, in which the delicate microstructure design of a stable material plays an important role. Herein, ZrNx barrier films with high amorphization are introduced in p-i-n perovskite solar cells. To quantify the amorphous-crystalline (a-c) density, pattern recognition techniques are employed. It is found the decreasing a-c interface in an amorphous film leads to dense atom arrangement and uniform distribution of chemical potential, which retards the interdiffusion at the interface between ions and metal atoms and protect the electrodes from corrosion. The resultant solar cells exhibit improved operational stability, which retains 88% of initial efficiency after continuous maximum power point tracking under 1-Sun illumination at room temperature (25 °C) for 1500 h.

Sensitive biosensors based on topological insulator Bi2Se3 and peptide.

In this work, we designed a facile and label-free electrochemical biosensor based on intrinsic topological insulator (TI) Bi2Se3 and peptide for the detection of immune checkpoint molecules. With topological protection, Bi2Se3 could have robust surface states with low electronic noise, which was beneficial for the stable and sensitive electron transport between electrode and electrolyte interface. The peptides are easily synthesized and chemically modified, and have good biocompatibility and bioavailability, which is a suitable candidate as the recognition units for immune checkpoint molecules. Therefore, the peptide/Bi2Se3 was developed as a suitable working electrode for the electrochemical biosensor. The basic performance of the designed peptide/Bi2Se3 biosensor was investigated to determine the Anti-HA Tag Antibody and PD-L1 molecules. The linear detection range was from 3.6 × 10-10 mg mL-1 to 3.6 × 10-5 mg mL-1, and the detection limit was 1.07 × 10-11 mg mL-1. Moreover, the biosensor also displayed good selectivity and stability.

Topological insulator Bi2Se3 based electrochemical aptasensors for the application of sensitive detection of interferon-γ.

Interferon-γ (IFN-γ) is one of the crucial inflammatory cytokines as an early indicator of multiple diseases. A fast, simple, sensitive and reliable IFN-γ detection method is valuable for early diagnosis and monitoring of treatment. In this work, we creatively developed an electrochemical aptasensor based on the topological material Bi2Se3 for sensitive IFN-γ quantification. The high-quality Bi2Se3 sheet was directly exfoliated from a single crystal, which immobilized the synthesized IFN-γ aptamer. Under optimal conditions, the electrochemical signal revealed a wide linear relation along with the logarithmic concentration of IFN-γ from 1.0 pg mL-1 to 100.0 ng mL-1, with the limit of detection as low as 0.5 pg mL-1. The topological material Bi2Se3 with Dirac surface states improved the electrochemical signal/noise ratio and thus the sensitivity of the sensors. Furthermore, this electrochemical aptasensor exhibited excellent specificity and stability, which could be attributed to the large-scale smooth surface of the Bi2Se3 sheet with few defects decreasing the non-specific absorption. The developed biosensor has the same good performance as the ELISA method for detecting the real serum samples. Our work demonstrates that the developed electrochemical aptasensors based on topological materials have great potential in the field of clinical determination.

Initializing film homogeneity to retard phase segregation for stable perovskite solar cells.

The mixtures of cations and anions used in hybrid halide perovskites for high-performance solar cells often undergo element and phase segregation, which limits device lifetime. We adapted Schelling's model of segregation to study individual cation migration and found that the initial film inhomogeneity accelerates materials degradation. We fabricated perovskite films (FA1-xCsxPbI3; where FA is formamidinium) through the addition of selenophene, which led to homogeneous cation distribution that retarded cation aggregation during materials processing and device operation. The resultant devices achieved enhanced efficiency and retained >91% of their initial efficiency after 3190 hours at the maximum power point under 1 sun illumination. We also observe prolonged operational lifetime in devices with initially homogeneous FACsPb(Br0.13I0.87)3 absorbers.

Reversible Phase Transition for Durable Formamidinium-Dominated Perovskite Photovoltaics.

Phase instability is one of the major obstacles to the wide application of formamidinium (FA)-dominated perovskite solar cells (PSCs). An in-depth investigation on relevant phase transitions is urgently needed to explore more effective phase-stabilization strategies. Herein, the reversible phase-transition process of FA1- x Csx PbI3 perovskite between photoactive phase (α phase) and non-photoactive phase (δ phase) under humidity, as well as the reversible healing of degraded devices, is monitored. Moreover, through in situ atomic force microscopy, the kinetic transition between α and δ phase is revealed to be the "nucleation-growth transition" process. Density functional theory calculation implies an enthalpy-driven α-to-δ degradation process during humidity aging and an entropy-driven δ-to-α healing process at high temperatures. The α phase of FA1- x Csx PbI3 can be stabilized at elevated temperature under high humidity due to the increased nucleation barrier, and the resulting non-encapsulated PSCs retain >90% of their initial efficiency after >1000 h at 60 °C and 60% relative humidity. This finding provides a deepened understanding on the phase-transition process of FA1- x Csx PbI3 from both thermodynamics and kinetics points of view, which also presents an effective means to stabilize the α phase of FA-dominated perovskites and devices for practical applications.

Enhanced Air and Electrochemical Stability of Li7P2.9Ge0.05S10.75O0.1 Electrolytes with High Ionic Conductivity for Thiophosphate-Based All-Solid-State Batteries.

Sulfide solid electrolytes (SSEs) show tremendous potential to realize high-energy-density secondary batteries and offer distinguishing safety features over the traditional liquid-electrolyte-based system. However, their installation is hindered by the air sensitivity and substandard interfacial compatibility with Li-metal anodes. Herein, an aliovalent P5+/Ge4+ and isovalent S2-/O2- cosubstitution strategy increases the σLi+ to 4.77 mS cm-1, which is associated with the lowest activation energy (18.66 kJ mol-1). Impressively, with limited substitution of P/Ge and S/O in Li7P3S11, the derived electrolytes largely suppressed the structural hydrolysis in the air. Furthermore, the Li//Li cell with novel Li7P2.9Ge0.05S10.75O0.1 SSEs realized Li plating/stripping over 100 h at 0.1 mA cm-2/0.1 mAh cm-2 @ RT, with the lowest overpotential at ∼5 mV. Next, ex situ X-ray photoelectron spectroscopy (XPS) quantified the electrochemical decomposition of the Li7P3S11/LiNbO3@NCA interface during cell operation. XPS results confirmed better thermodynamic stability between LiNbO3@NCA and L7P3S11 after GeO2 substitution. Accordingly, the LiNbO3@NCA/Li7P2.9Ge0.05S10.75O0.1/Li-In cell performed remarkably; first discharge capacity, 158.9 mAh g-1; capacity retention, 89%; and Coulombic efficiency, ∼100% after 50 cycles @ 0.064 mA cm-2 and even at 0.3 mA cm-2 versus the first discharge capacity and retention (129.4 mAh g-1 and 75.73%) after 70 cycles @ RT. These remarkable results could be attributable to the excellent σLi+, chemical/electrochemical stability toward LiNbO3@NCA, and meager interfacial resistance, essential for the practical application of sulfide-based batteries.

Surface-capping engineering for electrically neutral surface of perovskite films and stable solar cells.

Metal halide perovskite solar cells (PSCs) have developed rapidly in recent years, due to their high performance and low-cost solution-based fabrication process. These excellent properties are mainly attributed to the high defect tolerance of polycrystalline perovskite films. Meanwhile, these defects can also facilitate ion migration and carrier recombination, which cause the device performance and the long-term stability of PSCs to deteriorate heavily. Therefore, it is critical to passivate the defects, especially at the surfaces of perovskite grains where the defects are most concentrated due to the dangling bonds. Here we propose a surface-capping engineering (SCE) method to construct 'dangling-bond-free' surfaces for perovskite grains. Diamine iodide (methylenediammonium diiodide, MDAI2) was used to construct an electroneutral PbX6-MDA-PbX6(X = Cl, Br or I) layer at the perovskite surfaces. Compared to the monovalent FA+which can only coordinate one [PbX6]4-slab, the bivalent MDA2+can coordinate two [PbX6]4-slabs on both sides, thus realizing a dangling-bond-free surface. Solar cells based on SCE-perovskite films exhibited a higher power conversion efficiency (PCE) of 21.6%, compared with 19.9% of the control group; and maintained over 96% of its initial PCE after 13 h during the maximum power point tracking test under continuous AM1.5G illumination, whereas the control group only lasted 1.5 h. Constructing a dangling-bond-free capping layer on the grain boundary opens new avenues for the fabrication of ultralow-defect polycrystalline semiconductors, paving the way to further improve the PCE and lifetime of PSCs.

Dual-Layered Interfacial Evolution of Lithium Metal Anode: SEI Analysis via TOF-SIMS Technology.

Lithium metal battery has been considered as one of the most promising candidates for the next generation of energy storage systems due to its high energy density. However, the lithium metal may react with the electrolyte, resulting in the instability of the solid/liquid interface. The solid electrolyte interface (SEI) layer was found to affect the interface stability of the lithium metal anode; the real structure of SEI couldn't be accurately analyzed so far. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) has been thought as a powerful tool to carry out three-dimensional (3D) characterization and structural reconstruction at a high-resolution nanoscale, as well as detect ionized elements and molecule fragments at the ppb level due to its excellent sensitivity. Herein, we employed TOF-SIMS to investigate the chemical composition of SEI at the surface of the lithium metal anode after electrochemical cycles. We find that SEI is not a completely dense interface layer. The organic phase of SEI can accommodate part of the electrolyte, enhancing the lithium-ion conductivity. Meanwhile, SEI is an interface layer that changes with the state of the electrolyte, and this process of change is expressed by conventional characterization methods. However, the distribution of lithium salt can be analyzed by TOF-SIMS to judge the change degree of SEI. Our work provides significant guidance for accurately characterizing the SEI layer, as well as constructing a more realistic interface layer model.

Avoiding Structural Collapse to Reduce Lead Leakage in Perovskite Photovoltaics.

Perovskite solar cells (PSCs) have become a promising candidate for the next-generation photovoltaic technologies. As an essential element for high-efficiency PSCs however, the heavy metal Pb is soluble in water, causing a serious threat to the environment and human health. Due to the weak ionic bonding in three-dimensional (3D) perovskites, drastic structure decomposition occurs when immersing the perovskite film in water, which accelerates the Pb leakage. By introducing the chemically stable Dion-Jacobson (DJ) 2D perovskite at the 3D perovskite surface, the film dissolution is significantly slowed down, which retards lead leakage. As a result, the Pb contamination is dramatically reduced under various extreme conditions. In addition, the PSCs device deliver a power conversion efficiency (PCE) of 23.6 % and retain over 95 % of their initial PCE after the maximum power point tracking for over 1100 h.

Precise Control of a Yolk-Double Shell Metal-Organic Framework-Based Nanostructure Provides Enhanced Fire Safety for Epoxy Nanocomposites.

Nanomaterials derived from metal-organic frameworks (MOFs) are highly promising as future flame retardants for polymeric materials. The precise control of the interface for polymer nanocomposites is taking scientific research by storm, whereas such investigations for MOF-based nanofillers are rare. Herein, a novel yolk-double shell nanostructure (ZIF-67@layered double hydroxides@polyphophazenes, ZIF@LDH@PZS) was subtly designed and introduced into epoxy resin (EP) as a flame retardant to fill the vacancy of yolk/shell construction in the field. Meanwhile, the interface of the polymer nanocomposites can be further accurately tailored by the outermost layer of the nanofillers from PZS to Ni(OH)2 (NH), by which hollow nanocages with treble shells (LDH@PZS@NH) were obtained. It is remarkably interesting that LDH@PZS@NH endows the EP with the lowest peak of heat release rate in the cone calorimeter test, but the total heat and smoke releases (THR and TSP) of the nanocomposites are even higher than those of the neat polymer. In contrast, EP blended with ZIF@LDH@PZS shows outstanding comprehensive performance: with 2 wt.%, the limiting oxygen index is increased to 29.5%, and the peak heat release rate is reduced by 26.0%. The impact and flexural strengths are slightly lowered, while the storage modulus is enhanced remarkably compared with that for neat EP. The flame retardant mechanism is systematically explored focusing on the interfacial interactions of different hybrids within the epoxy matrix, ushering in a new stage of study of nanostructural design-guided interface manipulation in MOF-based polymer nanocomposites.

Electrochemical DNA Biosensors Based on the Intrinsic Topological Insulator BiSbTeSe2 for Potential Application in HIV Determination.

In this work, we reported a sensitive, label-free electrochemical biosensor based on the intrinsic topological insulator (TI) BiSbTeSe2 for potential application in the determination of the HIV gene. With strong spin-obit coupling, TIs could have robust surface states with low electronic noise, which might be beneficial for the stable and sensitive electron transport between the electrode and electrolyte interface. Under optimized conditions of the biosensors using BiSbTeSe2, the differential pulse voltammetry (DPV) peak currents showed a linear relationship with the logarithm of target DNA concentrations ranging from 1.0 × 10-13 to 1.0 × 10-7 M, with a detection limit of 1.07 × 10-15 M. The sensing assay also displayed good selectivity and stability after storage at 4 °C for 7 days. This work provides an effective way to develop biosensors with topological materials, which have a potential application in the clinical determination and monitoring field.

A cross-linked charring strategy for mitigating the hazards of smoke and heat of aluminum diethylphosphonate/polyamide 6 by caged octaphenyl polyhedral oligomeric silsesquioxanes.

Aluminum diethylphosphonate (ADP) is a highly efficient phosphorus-based flame retardant, widely used in polyamide 6 (PA6). However, ADP/PA6 releases large amounts of heat and smoke under high heat flux, which commonly means serious hazards to life and property. Octaphenyl polyhedral oligomeric silsesquioxanes (OPS) is an organic-inorganic hybrid silicon compound, playing flame retardant role in condensed phase. In this work, combustion behaviors of OPS/ADP/PA6 were investigated by limited oxygen index (LOI), UL94 and cone calorimeter (CONE) tests. The LOI and UL94 rating results did not change obviously, while the CONE data and smoke density data showed the synergistic effect of OPS and ADP in PA6. For 2.5%OPS/7.5%ADP/PA6, the peak values of heat, smoke and CO release rate (pk-HRR, pk-RSR, Ds, max with/without pilot flame and pk-COP) decreased by 60.2%, 82.1%, 45.9%/38.3% and 80.4% respectively, compared with 10%ADP/PA6. Moreover, 2.5%OPS/7.5%ADP/PA6 produced 337.5% more residue than 10%ADP/PA6. TGA, TG-IR, SEM-EDS, XPS and py-GC/MS were used to further explore the synergistic mechanism of OPS and ADP. It was verified that the cross-linked charring strategy apparently has weakened the hazards of smoke and heat of PA6. This work proposed a possible technical approach to solve both fire risk and heat/smoke hazards of PA6.

Enhanced Hydrogen Generation Performance of Al-Rich Alloys by a Melting-Mechanical Crushing-Ball Milling Method.

The main problem for the application of hydrogen generated via hydrolysis of metal alloys is the low hydrogen generation rate (HGR). In this paper, active Al alloys were prepared using a new coupled method-melting-mechanical crushing-mechanical ball milling method to enhance the HGR at room temperature. This method contains three steps, including the melting of Al, Ga, In, and Sn ingots with low melting alloy blocks and casting into plates, then crushing alloy plate into powders and ball milling with chloride salts such as NiCl2 and CoCl2 were added during the ball milling process. The microstructure and phase compositions of Al alloys and reaction products were investigated via X-ray diffraction and scanning electron microscopy with energy dispersed X-ray spectroscopy. The low-melting-point Ga-In -Sn (GIS) phases contain a large amount of Al can act as a transmission medium for Al, which improves the diffusion of Al to Al/H2O reaction sites. Finer GIS phases after ball milling can further enhance the diffusion of Al and thus enhance the activity of Al alloy. The hydrogen generation performance through hydrolysis of water with Al at room temperature was investigated. The results show that the H2 generation performance of the Al-low-melting point alloy composite powder is significantly higher than the results reported to date. The highest H2 generation rate and H2 conversion efficiency can reach 5337 mL·min-1·g-1 for the hydrolysis of water with 1 g active alloy.

Boosting Sodium Storage Performance of Hard Carbon Anodes by Pore Architecture Engineering.

Hard carbon (HC) displays great potential for high-performance sodium-ion batteries (SIBs) due to its cost-effective, simple fabrication and most likely to be commercialized. However, the complicated microstructures of HC lead to difficulties in deeply understanding the structure-performance correlation. Particularly, evaluation of influence of pore structure on Na storage performances is still causing disputes and rational strategies of designing pore architecture of HC are still necessary. In this work, the skillful and controllable phase-inversion method is applied to construct porous HC with abundantly interconnected and permeable tunnel-like pores, which can promote ionic diffusion and improve electrode-electrolyte interfacial affinity. Structure-performance investigation reveals that porous HC with cross-coupled macropore architecture can boost Na storage performances comprehensively. Compared to pristine HC with negligible pores, well-regulated porous HC anodes show an obvious enhancement on initial Coulombic efficiency (ICE) of 68.3% (only 51.5% for pristine HC), reversible capacity of 332.7 mAh g-1 at 0.05 A g-1, rate performance with 67.4% capacity retention at 2 A g-1 (46.5% for pristine HC), and cycling stability with 95% capacity maintained for 90 cycles (86.4% for pristine HC). Additionally, the ICE can be optimized up to 76% by using sodium carboxymethyl cellulose as a binder. This work provides an important view of optimizing Na storage performances of HC anodes by pore engineering, which can be broadened into other electrode materials.