The low concentration of CO2 in industrial emissions (similar to 10 %) makes its direct utilization for CO2 electrocatalytic reduction (CO2RR) challenging. This study presents an integrated approach combining CO2 enrichment with electrocatalytic reduction to address this limitation. A highly efficient solid amine adsorbent (RFCA-65 %PEI) was developed, leveraging mesoporous carbon to achieve a CO2 adsorption capacity of 185 mgg(-1) and enrich CO2 from 10 % to 42 % under optimized conditions. The enriched CO2 was then converted via a Ni single-atom catalyst (Ni-NMC), which exhibited exceptional selectivity, increasing the Faradaic efficiency (FECO) from 75 % to 92.3 % at -0.73 V (vs. RHE) in an H-cell. Further optimization revealed that electrolyte composition and gas flow rate critically influence the performance. Using 0.2 M KOH and a 20 mLmin(-1) inlet flow rate in a flow cell, Ni-NMC achieved FECO >95 % at 150 mAcm(-2), while maintaining >90 % efficiency over 18 h. In addition, the role of HCO3- in buffering local pH and suppressing competing hydrogen evolution was highlighted. This work not only demonstrates a viable pathway for industrial low-concentration CO2 valorization but also provides insights into the synergistic design of adsorption-electrocatalysis systems for sustainable carbon management.

Lithium-sulfur (Li-S) batteries are regarded as promising candidates for next-generation high-energy storage systems due to their superior theoretical capacity. However, their commercial application is severely constrained by the polysulfide shuttle effect and slow reaction kinetics. This study synthesized a g-C3N4-based heterostructured separator modification material, g-C3N4-MoS2/VS2 (MoVSCN), via a two-step hydrothermal method. The material not only facilitates spontaneous electron redistribution at the ternary interfaces, forming an internal electric field and abundant defect sites for effective adsorption and catalysis of polysulfides, but also achieves a synergistic optimization of electron and ion transport pathways, thereby significantly enhancing the overall reaction kinetics and cycling stability of lithium-sulfur batteries. Electrochemical testing indicates that the modified battery exhibits high capacity (1353 mAh g-1 during initial discharge at 0.2 C), excellent rate performance (721 mAh g-1 at 5 C), and exceptionally long lifespan (capacity decay rate of only 0.048% after 1000 cycles at 1 C). Even under low-temperature conditions (0 degrees C), the battery maintains a high specific capacity of 1160.7 mAh g-1 and an impressive capacity retention of 83.6%. The morphology of the lithium anode after cycling demonstrates its ability to nearly completely suppress the shuttle effect. These findings lay a solid foundation for pioneering advances in ternary composite materials and heterostructure interface engineering.

Due to their exceptional electrochemical properties, lithium-sulfur batteries are regarded as one of the most promising candidates for energy storage systems. Yet, their commercialization is significantly hindered by severe shuttle effects and sluggish redox kinetics. Herein, a highly ordered mesoporous TiO2 (OMT) material with atomic-level Nb doping (Nb-OMT) was innovatively constructed as a bifunctional electrocatalyst, enabling superior performance in lithium‑sulfur (LiS) batteries. Density functional theory (DFT) calculations confirm that Nb doping could effectively enhance the electrical conductivity of the mesoporous TiO2, facilitating simultaneous adsorption and catalytic conversion of lithium polysulfides (LiPSs) on the material surface, thereby accelerating sulfur redox kinetics. Therefore, the LiS cell with Nb-OMT-20 modified separator demonstrates an exceptional specific capacity of 1348.9 mAh g-1 in LiS batteries at 0.2C, meanwhile exhibiting an ultralow capacity decay rate of merely 0.036% per cycle over 900 cycles at 1C. Notably, even under challenging conditions, including a high sulfur loading of 5.12 mg cm-2 and a low temperature of 273 K, the LiS battery still delivers a considerable capacity of 1146.1 mAh g-1 at 0.1C with a capacity retention of 83.4% of its capacity over 100 cycles at 0.2C, suggesting promising potential for practical applications. This work presents a novel approach to developing bifunctional electrocatalysts through atomic-scale structural modulation, thereby advancing the industrial application of LiS batteries.

Removal of hydrogen sulfide (H2S) over carbon catalysts at room temperature is affected by catalytic activity, mass transfer efficiency and product storage space. In this work, nitrogen-doped mesoporous carbon with different morphologies was prepared under the induction of structure-directing agents. The desulfurization performance of the desulfurizers was evaluated after loading with sodium hydroxide (NaOH). Among them, the impregnated alkaline species promotes the dissociation of H2S. It is noteworthy that the nitrogen-doped carbon nanosheet exposes more defective sites. This facilitates the activation of oxygen, which in turn improves the catalytic ability. Meanwhile, the combination of carbon nanosheets and mesopores not only shortens the pathway for substance diffusion, but also provides additional space for product storage. Therefore, the alkaline nitrogen-doped carbon nanosheet desulfurizers (i.e. NCS-30) achieves an excellent breakthrough capacity of 7.13 g/g. Further, the in-situ DRIFT result reveals that the nitrogen atom in the carbon skeleton is one of the core catalytic active sites. Based on the experimental results, a possible mechanism for the catalytic oxidation of H2S over alkaline nitrogen-doped mesoporous carbon desulfurizers at room-temperature is submitted. This work provides a seemingly feasible idea for the design of high-performance carbon-based desulfurizers and the refinement of existing desulfurizers.

Ni single-atom catalysts have been widely explored for CO2 reduction, however, their practical application is often hampered by complex synthesis and instability at high current densities. In this context, well-dispersed nickel nanoparticles present a compelling alternative, offering both facile fabrication and robust performance. Herein, a hierarchical catalyst comprising nickel nanoparticles encapsulated within a nitrogen-doped carbon shell on a hollow-rod carbon substrate (denoted as NiNP-BCN@C) was designed. The hollow-rod architecture maximizes the exposure of nickel nanoparticles as active sites, while the nitrogen-doped carbon shell effectively modulates the electronic environment of the metallic Ni, suppressing the competing hydrogen evolution reaction and promoting CO2 activation. The catalyst exhibits exceptional CO2-to-CO conversion, with a Faradaic efficiency exceeding 90

In this work, a high-entropy oxide catalyst uniformly anchored on reduced graphene oxide is developed with diverse active sites to promote lithium polysulfide conversion and suppress the shuttle effect. Such a separator coating endows lithium-sulfur batteries with outstanding high-loading performance (3.8 mAh cm-2) and low-temperature behavior (95% capacity retention at 0 degrees C after 100 cycles).

Aqueous zinc-metal batteries offer significant advantages in terms of safety and cost, yet they remain constrained by large desolvation energy barrier of the bulky [Zn(H2O)6]2+ solvation clusters, leading to issues such as dendrite growth and side reactions. To overcome these challenges, a two-dimensional ordered-mesoporous covalent organic framework with electron-delocalized characteristics (2D mCOF) is developed as an interfacial catalyst layer to inhibit undesirable parasitic reactions and modulate Zn2+ flux. Serving as an interfacial kinetic accelerator, the 2D mCOF promotes Zn2+ dissociation through the size-screening effect of their intrinsic microporous structure and the strong Zn2+ affinity of surface functional groups. Simultaneously, the mesoporous structure enables rapid Zn2+ transport under high current densities. The incorporation of electron-withdrawing cyano groups (-CN) within the framework further enhances local electron delocalization, boosting the electrocatalytic activity of the COF and accelerating desolvation kinetics, as supported by theoretical simulations, Raman spectroscopic analyses, and detailed electrochemical tests. Remarkably, under extreme low-temperature conditions, Zn symmetric cell with the 2D mCOF promoter demonstrates an exceptional long-term cycling stability, operating reliably for over 4500 h at 0.5 mA cm-2. Moreover, when assembled into a full cell, an impressive capacity retention of 97.1% is maintained after 4000 cycles at 20 A g-1, highlighting the strong potential of 2D mCOF for enabling high-performance low-temperature aqueous zinc-metal batteries.

Catalytic oxidation of hydrogen sulfide (H2S) at room temperature enables deep desulfurization and efficient recovery of elemental sulfur. Base-loading and N-doping are major modification strategies for carbon-based catalysts, while comparative research on their respective roles in carbon substrates and basic sites remains insufficient. Herein, silica-nanocasting on agarose hydrogel is adopted to fabricate highly mesoporous carbon aerogels with the modification of MgO-loading (MCAs) or urea co-pyrolysis (NCAs). Precise MgO regulation and ultra-high N doping of 23.1 wt% enhance aerogels to achieve excellent sulfur capacities of 3.38 and 0.90 g H2S g-1 depends only on nitrogen doping content. MgO-modified carbon alleviates sulfur blockage via water refreshing theory, yet its strong O2 activation capacity easily induces overoxidation. Nitrogen-doped carbon features mild oxygen activation, but suffers active site loss from strong S8 adsorption. DFT calculations indicate that H2S adsorption on the MgO surface is weak, whereas its dissociation energy barrier is extremely low. Pyrrolic and pyridinic N exhibit completely opposite behavior toward H2S compared with MgO. This study elucidates the catalytic oxidation mechanisms of the two modification strategies, providing a solid foundation for integrating their advantages to construct efficient desulfurization catalysts. cat, respectively. Performance of MCAs is constrained by pore volume and loading, while that of NCAs

Silicon-based anodes for lithium-ion batteries are hindered by the large volume expansion and low intrinsic conductivity of silicon. To overcome these issues, petroleum coke-derived silicon-carbon microspheres doped with transition metals (V, Mn, and Ni) were prepared via a one-step spray-drying method. In this configuration, nano-silicon functions as the active core for a high capacity, while an artificial graphite (AG) framework derived from petroleum coke provides conductive pathways and accommodates volume changes. Transition metal doping further introduces additional lithium storage sites and improves electronic conductivity. The optimized Mn-doped material (0.3%Mn@AG-Glu-Si) exhibits outstanding cycling stability, delivering an initial discharge capacity of 1803.2 mAh g(-1) and retaining 1245.9 mAh g(-1) after 100 cycles at 0.5 A g(-1). Furthermore, during the activation phase, it demonstrates a high initial discharge capacity of 2093.6 mAh g(-1) with a Coulombic efficiency of 86.64% at 0.1 A g(-1), confirming its high lithium storage capability. Mechanism analysis reveals that Mn doping strengthens the binding energy (-6.83 eV) and Li+ adsorption energy (-3.1 eV), as well as improves electron transport by increasing the density of states near the Fermi level. This work presents a practical and effective strategy for developing high-performance silicon-based anode materials.

With heat dissipation and electromagnetic interference (EMI) caused by the integration of electronic elements becoming more serious, developing thermal interface materials (TIMs) with higher thermal conductivity, and EMI shielding performance is urgent. An anisotropic polyimide/mesocarbon microbeads/graphene oxide/polymer composite bifunctional material (PDMS/PMGO) has been successfully prepared by the directional freezing method and multistep high-temperature thermal annealing. PDMS/PMGO has high through-plane thermal conductivity (7.191 W & centerdot;m-1 & centerdot;K-1), excellent EMI shielding performance (high absorption loss of 68.66 dB and electromagnetic shielding efficiencies of 77.46 dB), good mechanical strength, thermal stability properties, and compressive strength. PDMS/PMGO has the potential to be used as a new generation of TIMs and electromagnetic shielding materials in high frequency electronic devices, aerospace and smart wearable devices.

Hard carbon materials are considered among the most promising anodes for sodium-ion batteries owing to their abundant precursors, low cost, and suitable sodium storage potential. However, their practical application is hindered by low initial Coulombic efficiency, poor rate capability, and inadequate interfacial stability. A dual-carbon synergistic design strategy using polyvinylidene chloride (PVDC) and phenolic resin is proposed. A highly closed-cell carbon (V18-1450) is prepared from PVDC via pre-carbonization and high-temperature carbonization. Subsequently, phenolic resin coating via liquid-phase ball milling and carbonization forms a core-shell composite V18-1450@20RF. The resin-derived carbon coating repairs surface defects, promotes the conversion of open pores to closed pores, and reduces the specific surface area. Benefiting from such nanoscale interfacial regulation, the optimized V18-1450@20RF anode exhibits a reversible specific capacity of 405.9 mAh g−1 at 30 mA g−1, along with an initial Coulombic efficiency (ICE) of 84.49%. After 500 cycles at 1500 mA g−1, the capacity retention remains as high as 88.72%. Notably, it maintains an excellent specific capacity of 233.2 mAh g−1 even under harsh conditions of −20 °C and a high rate of 3000 mA g−1. Kinetic analysis confirms that the sodium storage mechanism follows a multistep "adsorption-intercalation-pore filling" model, with the carbon coating significantly enhancing Na+ diffusion kinetics. This study demonstrates that the synergistic design of PVDC-derived hard carbon with a phenolic resin-derived carbon coating offers a promising strategy for developing sodium-ion battery anodes with high capacity, high initial Coulombic efficiency, and superior rate capability.

Transition metal oxides like Co3O4 are promising for CO oxidation but suffer from severe deactivation in humid environments. Herein, the highly active and water-resistant Co3O4/C composite catalyst (Co3O4-N180A) was synthesized via a surfactant-assisted solvothermal method followed by a two-step calcination strategy. This approach preserves a hierarchical porous nanosheet structure with high specific surface area (36.4 m2·g−1), enriched surface Co3+ species (58.5%), and abundant oxygen vacancies. The Co3O4-N180A catalyst exhibits exceptional activity, achieving complete CO conversion at 130 ℃ under a high GHSV of 120,000 mL·h−1·gcat−1. Moreover, Co3O4-N180A demonstrates outstanding water-resistance, maintaining a steady 100% CO conversion at 170 ℃ in the presence of 10 vol% H2O. FTIR spectroscopy, water contact angle measurements and DFT calculations reveal that the residual amorphous carbon matrix functions as a water-resistant shield. This weak water affinity (Eads(Co3O4/C-H2O) of −0.92 eV) prevents the competitive adsorption of H2O and protects the Co3+ active sites from detrimental surface hydroxylation. This work provides a structural engineering strategy for developing robust, water-resistant catalysts for CO oxidation at low temperatures.

Low-temperature SCR denitrification technology requires catalysts with both NOx oxidation and NH3 adsorption capabilities. However, most catalysts, such as MnOx and MnO2/TiO2, with the problems of narrow activity temperature windows and low sulfur resistance. Herein, the mesoporous amorphous oxide catalysts Sm alpha-MnTiOx are successfully synthesized by a solvothermal method. The catalyst displays excellent low-temperature activity and sulfur tolerance, with a denitrification conversion of over 90 % within the range of 160 degrees C to 350 degrees C. Furthermore, the denitrification conversion wasis maintained at more than 98 % for 8 h at 250 degrees C and 50 ppm SO2 atmosphere. The reducibility capacity and surface acidity of Sm alpha-MnTiOx catalysts are improve by the doping of Sm, thus facilitating the adsorption and activation of NH3 and O2, which is beneficial for the improvement of catalytic activity. The in-situ DRIFTS shows the abundant chemisorbed oxygen on the surface of Sm alpha-MnTiOx favors NO2 generation, and the doping of Sm extended the temperature range of NO2 (50-250 degrees C), which promotes the reaction towards the Fast-SCR reaction pathway at low temperatures. The combined effect of E-R mechanism and Fast-SCR reaction successfully broaden the denitration temperature window of Sm alpha-MnTiOx catalysts. Furthermore, the interaction between Mn and Sm species effectively inhibits the electron transfer from Mn to SO2, which reduces the generation of metal sulfate and protects the active sites of the catalyst. This study provides new ideas for the improvement of denitrification catalysts with sulfur tolerance, water resistance and upper and lower catalytic activity.

It remains a great challenge to improve the low-temperature SO2 resistance of catalysts applied for selective catalytic reduction of NOx with NH3 (NH3-SCR). This work develops an outstanding SO2-tolerant Fe-Ti (FT) catalyst by W/SO42- co-modification via a sol-gel method using Fe(NO3)(3)9H(2)O, tetrabutyl titanate, ammonium tungstate and thiourea as raw materials. The physicochemical characterizations, in-situ diffuse reflectance infrared Fourier transform (DRIFT) measurements and density functional theory (DFT) calculations were combined to reveal the underlying mechanisms. Although W doping can effectively enhance the surface acidity, NH3 adsorption on Lewis acid sites can still be restrained by competitive adsorption of SO2, whereas SO42- modification can enhance the adsorption stability of NH3 without being affected by SO2. Simultaneously, the NO adsorption ability on Fe sites can be significantly enhanced by W/SO42- co-modification. Furthermore, the W doping or SO42- modification can induce conversion of Fe3+ to Fe2+ to affect the redox property of Fe species. A proper amount of Fe2+ suppressed the oxidizability of FT catalyst to inhibit NH3 overoxidation to enhance N-2 selectivity, and created more oxygen vacancies to generate larger amount of chemisorbed oxygen to facilitate NH3 dehydrogenation and NO oxidation. More importantly, the inhibition effect of SO2 adsorption on Fe sites was strengthened by W/SO42- co-modification. Consequently, the W/SO42- co-modified FT catalyst exhibited high activity with >90 % of NO conversion and >95 % of N-2 selectivity within a broad window of 275-450 degrees C and possessed superior SO2 + H2O tolerance at 275 degrees C.

The precise atomic-scale preparation of single-atomic active sites with unique coordination structures in electrocatalysts for the carbon dioxide reduction reaction (CO2RR), coupled with the elucidation of their mechanisms at the atomic level, remains a formidable challenge. In this manuscript, a simple one-pot synthesis method was adopted to successfully synthesize an O-doped Ni single-atom catalyst (Ni-NOG), characterized by a distinct Ni-N2O2 symmetric coordination structure. The incorporation of Ni-O bonds alters the electronic configuration of the catalyst's central atoms within the catalyst, thereby boosting both the catalytic selectivity and efficiency during CO2RR. The synthesized electrocatalyst exhibited outstanding performance in the CO2RR process, achieving a Faraday efficiency (FE) of 97.4 % at a potential of -0.8315 V versus to reversible hydrogen electrode (vs. RHE). Furthermore, the selectivity remained consistently above 95 % throughout a 98-hour stability test, surpassing the performance of most advanced catalysts currently available. Theoretical simulations demonstrate that the Ni-N2O2 symmetric coordination structure shows a small activation barrier in the rate-limiting step, favoring the swift generation of intermediate species and demonstrating robust catalytic activity. This work not only offers a straightforward and approach method for the preparation of single-atom catalysts but also clarifies the pivotal role of O-element doping within the coordination environment in enhancing catalyst performance.

Extensive research has been conducted on the selective catalytic oxidation of hazardous H2S to elemental sulfur at room temperature using base-loaded carbon catalysts. However, practical applications of these catalysts are hindered by economic and environmental constraints associated with the complex synthesis and activation of functional carbon substrates. Understanding the synergistic mechanism between carbon and bases is crucial for developing innovative catalysts with low carbon content. Herein, molecular simulations were first employed to elucidate the adsorption preferences and reaction pathways within the water film theory, confirming the carbon-MgO interface as the active catalytic site. Furthermore, the ultrathin hierarchically porous carbon layer was demonstrated to effectively mitigate catalyst deactivation by maintaining reaction channels and facilitating product diffusion. Guided by the theoretical insights, nanoflower catalysts were successfully constructed with precisely controlled carbon coating content. Remarkably, MgO@C-0.1 with only 16.7 wt % carbon content exhibited an exceptional sulfur capacity of 4.32 g H2S g-1 cat. This unprecedented carbon utilization efficiency stems from interfacial carbon defects, enhanced mass transport through the ultrathin carbon layer, and abundant sulfur storage space outside nanosheets. This study provides fundamental design principles for exploiting the catalytic potential of carbon and offers inspiring perspectives for developing high-performance catalysts with low carbon footprint.

Vanadium-based catalysts are considered an effective strategy to resolve the shuttle effect and sluggish solid-liquid-solid reaction kinetics in lithium-sulfur (Li-S) batteries, thanks to their strong adsorption and catalytic conversion capabilities toward polysulfides. Herein, a self-oxidation-driven solvothermal strategy was employed to construct a defect-rich homologous heterostructure of nanoflower-like VS2-VOx on a two-dimensional conductive V2C network (denoted as VSOC). The experimental results demonstrate that VSOC effectively enhances the multiphase redox reaction kinetics of sulfur species through the strong adsorption and spontaneous transformation of long-chain polysulfides by the highly conductive V2C and the accelerated catalytic reduction of insoluble short-chain Li2S by the V-S-O heterostructure. Consequently, the Li-S cells assembled with VSOC-modified separator and normal loaded 1.0 mg cm(-2) KB/S cathode deliver a high first discharge capacity of 1340 mAh g(-1) at 0.2 C with a low-capacity decay rate of 0.03% per cycle during long-term cycling at 1 C. It still achieves a capacity contribution of 501.3 mAh g(-1) even at 5 C. Moreover, under challenging conditions such as high sulfur loading (4.2 mg cm(-2)) and low temperature (0 degrees C), the VSOC-modified separator maintains 89% and 85% capacity retention and stable Coulombic efficiency. This study proposes a novel heterostructure design strategy for optimizing the performance of Li-S batteries.

Lithium-sulfur (Li-S) batteries are considered a promising alternative to conventional lithium-ion batteries due to their high theoretical capacity. However, the lithium polysulfide shuttle effect and inefficient redox kinetics impede their practical application. In this study, a 1T-VSe2@Ti3C2 heterostructure was rationally designed via a facile one-step hydrothermal method. The heterostructure, composed of conductive MXene and metallic 1T-VSe2, forms a built-in electric field that effectively promotes electron transport, which is beneficial for enhancing polysulfide adsorption and boosting sulfur conversion kinetics. Furthermore, a dynamic intercalation-conversion site (LixVSe2) improved lithium-ion transport and redox reversibility, which is confirmed by XPS analysis and in situ Raman spectroscopy. Therefore, Li-S cells with 1T-VSe2@Ti3C2-modified separators exhibited exceptional electrochemical performance, achieving an initial capacity of 1457 mAh g(- 1) with a high retention rate of 71%, a high-rate capability of 847 mAh g(- 1) at 4 C, and a durable cycle life with a capacity attenuation rate of 0.06% per cycle at 1 C over 1000 cycles. Notably, a reversible areal capacity of 4.8 mAh cm(- 2) is maintained under a high sulfur loading (5.5 mg cm(- 2)) after 100 cycles at 0.2 C. This work provides a universal strategy for constructing separator modifiers based on transition-metal selenides and highlights the potential of heterostructure engineering for achieving durable and practical Li-S batteries.

Aqueous zinc-ion batteries (AZIBs) hold significant promise for energy storage; however, the high dissociation energy barriers of bulky hydrated zinc ions ([Zn(H2O)6]2+) induce uneven Zn deposition, leading to severe capacity degradation and a limited cycle life. Herein, an effective desolvation-enhanced zinc anode protective layer is constructed using Mo4/3B2-X nanosheets, in which the etching-induced metal vacancies and -F zincophilic sites endow the layer with a strong affinity for Zn2+ and effectively catalyze the desolvation of [Zn(H2O)6]2+. Experimental and theoretical calculations demonstrate that under the action of Mo4/3B2-X , the desolvation energy of [Zn(H2O)6]2+ can be effectively reduced from 38.99 kJ mol-1 of bare Zn to 27.67 kJ mol-1, significantly promoting greater flux and rapid diffusion of free Zn2+. As a result, this configuration achieves a dendrite-free Mo4/3B2-X -Zn anode with an ultralong cycling life exceeding 2000 h, which is 18 times that of bare Zn. Even under low-temperature conditions at 0 degrees C, the Mo4/3B2-X -Zn anode maintains stable cycling for over 2800 h with a low overpotential of 58 mV at 0.5 mA cm-2. Pairing with the KVO cathode, the full cell delivers a capacity of up to 291.2 mA h g-1 at 0 degrees C and the pouch cell achieves 256.9 mA h g-1 under a high mass loading of 9.5 mg cm-2, demonstrating promising commercial potential.

Lithium‐sulfur (Li─S) batteries suffer from significant capacity degradation, which is limited by high barriers from interfacial desolvation, Li + transportation to sulfur redox conversions, exhibiting the depressive kinetics. Herein, the electron effect in the edge of catalysts is modulated and the corresponding strategy of self‐transform Schottky heterojunction on MXene is proposed to achieve the edge delocalized electronic density. As a protocol, the electron‐delocalized Schottky heterojunction of boron‐doped MXene/TiO 2 (SH‐MTB) is fabricated as electrochemical kinetic accelerators to realize fast Li + desolvation to promote rapid sulfur conversion kinetics under low‐temperature. Specifically, the Schottky heterojunction with edge effect expedites the dissociation kinetics of [Li(solvents) x ] + to generate free Li ions, as well‐confirmed by theoretical calculations and ex‐situ/in situ electrochemical characterizations. Encouragingly, higher practical areal capacity (5.0 mAh cm −2 ) and negligible self‐discharge behaviors are achieved under low‐temperature environments. A large areal pouch cell with 200 mg s exhibits 9.3 mAh cm −2 under a lean electrolyte amount (5 µL mg −1 ), much better than state‐of‐art reports. As further indicated by electronic microscopies, spectroscopical measurements and X‐ray tests, the SH‐MTB stabilizes the chemical structure during charge/discharge process, showing promising potential of Schottky heterostructure toward accelerating the cascade carrier kinetics in Li metal battery under low‐temperature.