Regulating Electron Filling and Orbital Occupancy of Anti-Bonding States of Transition Metal Nitride Heterojunction for High Areal Capacity Lithium-Sulfur Full Batteries.

The commercialization of lithium-sulfur (Li-S) battery is seriously hindered by the shuttle behavior of lithium (Li) polysulfide, slow conversion kinetics, and Li dendrite growth. Herein, a novel hierarchical p-type iron nitride and n-type vanadium nitride (p-Fe2 N/n-VN) heterostructure with optimal electronic structure, confined in vesicle-like N-doped nanofibers (p-Fe2 N/n-VN⊂PNCF), is meticulously constructed to work as "one stone two birds" dual-functional hosts for both the sulfur cathode and Li anode. As demonstrated, the d-band center of high-spin Fe atom captures more electrons from V atom to realize more π* and moderate σ* bond electron filling and orbital occupation; thus, allowing moderate adsorption intensity for polysulfides and more effective d-p orbital hybridization to improve reaction kinetics. Meanwhile, this unique structure can dynamically balance the deposition and transport of Li on the anode; thereby, more effectively inhibiting Li dendrite growth and promoting the formation of a uniform solid electrolyte interface. The as-assembled Li-S full batteries exhibit the conspicuous capacities and ultralong cycling lifespan over 2000 cycles at 5.0 C. Even at a higher S loading (20 mg cm-2 ) and lean electrolyte (2.5 µL mg-1 ), the full cells can still achieve an ultrahigh areal capacity of 16.1 mAh cm-2 after 500 cycles at 0.1 C.

Boosting the Energy Density of Bowl-Like MnO2@Carbon Through Lithium-Intercalation in a High-Voltage Asymmetric Supercapacitor with "Water-In-Salt" Electrolyte.

Highly concentrated "'water-in-salt"' (WIS) electrolytes are promising for high-performance energy storage devices due to their wide electrochemical stability window. However, the energy storage mechanism of MnO2 in WIS electrolytes-based supercapacitors remains unclear. Herein, MnO2 nanoflowers are successfully grown on mesoporous bowl-like carbon (MBC) particles to generate MnO2/MBC composites, which not only increase electroactive sites and inhibit the pulverization of MnO2 particles during the fast charging/discharging processes, but also facilitate the electron transfer and ion diffusion within the whole electrode, resulting in significant enhancement of the electrochemical performance. An asymmetric supercapacitor, assembled with MnO2/MBC and activated carbon (AC) and using 21 m LiTFSI solution as the WIS electrolyte, delivers an ultrahigh energy density of 70.2 Wh kg-1 at 700 W kg-1, and still retains 24.8 Wh kg-1 when the power density is increased to 28 kW kg-1. The ex situ XRD, Raman, and XPS measurements reveal that a reversible reaction of MnO2 + xLi+ + xe-↔LixMnO2 takes place during charging and discharging. Therefore, the asymmetric MnO2/MBC//AC supercapacitor with LiTFSI electrolyte is actually a lithium-ion hybrid supercapacitor, which can greatly boost the energy density of the assembled device and expand the voltage window.

Color-Tunable Perovskite Nanomaterials with Intense Circularly Polarized Luminescence and Tailorable Compositions.

The ability to design halide perovskite nanocrystals (PNCs) with circularly polarized luminescence (CPL) offers exceptional potential in photonic technologies. Despite recent inspiring advances, the creation of PNCs with full-color tailorablity, outstanding CPL, and long-term stability remains a substantial challenge. Herein, a robust strategy to craft CPL-active PNCs is reported, exhibiting appealing full-color tunable wavelengths, enhanced CPL, and prolonged stability. In contrast to conventional methodologies, this strategy utilizes chiral nematic mesoporous silica (CNMS) as host to render in situ confined growth of diverse achiral PNCs. By strategically engineering photonic bandgap, adjusting loading amount of PNCs, and manipulating cations/anion compositions of PNCs, robust CPL responses with tunable wavelength and intensity are successfully obtained. The resulting PNCs-CNMS achieves stable CPL emissions with full-color tunability and impressive luminescent dissymmetric factors up to -0.17. Remarkably, silica-based hosts as a protective barrier confer exceptional resistance to humidity, photodegradation, and thermal stability, even up to 95 °C. Furthermore, the ability to achieve reversible CPL switching within PNCs-CNMS is attainable by leveraging the responsiveness of CNMS matrix or dynamic behavior of impregnated PNCs. Additionally, circularly polarized light-emitting diode devices based on PNCs-CNMS can be conveniently fabricated. This research affords a powerful platform for designing functional chiroptical materials.

Honeycomb-Structured MoSe2 /rGO Composites as High-Performance Anode Materials for Sodium-Ion Batteries.

Sodium-ion batteries are a promising substitute for lithium batteries due to the abundant resources and low cost of sodium. Herein, honeycomb-shaped MoSe2 /reduced graphene oxide (rGO) composite materials are synthesized from graphene oxide (GO) and MoSe2 through a one-step solvothermal process. Experiments show that the 3D honeycomb structure provides excellent electrolyte penetration while alleviating the volume change during electrochemical cycling. An anode prepared with MoSe2 /rGO composites exhibits significantly improved sodium-ion storage properties, where a large reversible capacity of 215 mAh g-1 is obtained after 2700 cycles at the current density of 30.0 A g-1 or after 5900 cycles at 8.0 A g-1 . When such an anode is paired with Na3 V2 (PO4 )3 to form a full cell, a reversible specific capacity of 107.5 mAh g-1 can be retained after 1000 cycles at the current of 1.0 A g-1 . Transmission electron microscopy, X-ray photoelectron spectroscopy and in situ X-ray diffraction (XRD) characterization reveal the reversible storage reaction of Na ions in the MoSe2 /rGO composites. The significantly enhanced sodium storage capacity is attributed to the unique honeycomb microstructure and the use of ether-based electrolytes. This study illustrates that combining rGO with ether-based electrolytes has tremendous potential in constructing high-performance sodium-ion batteries.

Constructing a Stable Built-In Electric Field in Bi/Bi2Te3 Nanowires for Electrochemical CO2 Reduction Reaction.

Electrochemically converting carbon dioxide (CO2) into valuable fuels and renewable chemical feedstocks is considered a highly promising approach to achieve carbon neutrality. In this work, a robust interfacial built-in electric field (BEF) has been successfully designed and created in Bi/Bi2Te3 nanowires (NWs). The Bi/Bi2Te3 NWs consistently maintain over 90% Faradaic efficiency (FE) within a wide potential range (-0.8 to -1.2 V), with HCOOH selectivity reaching 97.2% at -1.0 V. Moreover, the FEHCOOH of Bi/Bi2Te3 NWs can still reach 94.3% at a current density of 100 mA cm-2 when it is used as a cathode electrocatalyst in a flow-cell system. Detailed in situ experiments confirm that the presence of interfacial BEF between Bi and Bi/Bi2Te3 promotes the formation of *OHCO intermediates, thus facilitating the production of HCOOH species. DFT calculations show that Bi/Bi2Te3 NWs increase the formation energies of H* and *COOH while reducing the energy barrier for *OCHO formation, thus achieving a bidirectional optimization of intermediate adsorption. This work provides a feasible scheme for exploring electrocatalytic reaction intermediates by using the BEF strategy.

Amorphization-Induced Cation Exchange in Indium Oxide Nanosheets for CO2-to-Ethanol Conversion.

Cation exchange (CE) in metal oxides under mild conditions remains an imperative yet challenging goal to tailor their composition and enable practical applications. Herein, we first develop an amorphization-induced strategy to achieve room-temperature CE for universally synthesizing single-atom doped In2O3 nanosheets (NSs). Density functional theory (DFT) calculations elucidate that the abundant coordination-unsaturated sites present in a-In2O3 NSs are instrumental in surmounting the energy barriers of CE reactions. Empirically, a-In2O3 NSs as the host materials successfully undergo exchange with unary cations (Cu2+, Co2+, Mn2+, Ni2+), binary cations (Co2+Mn2+, Co2+Ni2+, Mn2+Ni2+), and ternary cations (Co2+Mn2+Ni2+). Impressively, high-loading single-atom doped (over 10 atom %) In2O3 NSs were obtained. Additionally, Cu/a-In2O3 NSs exhibit an excellent ethanol yield (798.7 µmol g-1 h-1) with a high selectivity of 99.5% for the CO2 photoreduction. This work offers a new approach to induce CE reactions in metal oxides under mild conditions and constructs scalable single-atom doped catalysts for critical applications.

The Reconstruction of Bi 2 Te 4 O 11 Nanorods for Efficient and pH-universal Electrochemical CO 2 Reduction.

The practical application of electrochemical CO2 reduction reaction (CO2RR) is hindered by the competing CO production, hydrogen evolution reaction (HER), and the lack of pH-universal catalysts. Here, Te-modified Bi nanorods (Te-Bi NRs) were synthesized through in situ reconstruction of Bi2Te4O11 NRs under the CO2RR condition. Our study illustrates that the complex reconstruction process of Bi2Te4O11 NRs during CO2RR could be decoupled into three distinct steps, i.e., the destruction of Bi2Te4O11, the formation of Te/Bi phases, and the dissolution of Te. The thus-obtained Te-Bi NRs exhibit remarkably high performance in CO2RR towards formate production, showing high activity, selectivity, and stability across all pH conditions (acidic, neutral, and alkaline). In a flow cell reactor under neutral, alkaline, or acidic conditions, the catalysts achieved HCOOH Faradaic efficiencies of up to 94.3%, 96.4%, and 91.0%, respectively, at a high current density of 300 mA cm-2. DFT calculations, along with operando spectral measurements, reveal that Te manipulates the Bi sites to an electron-deficient state, enhancing the adsorption strength of the *OCHO intermediate, and significantly suppressing the competing HER and CO production. This study highlights the substantial influence of catalyst reconstruction under operational conditions and offers insights into designing highly active and stable electrocatalysts towards CO2RR.

Two-dimensional Cu Plates with Steady Fluid Fields for High-rate Nitrate Electroreduction to Ammonia and Efficient Zn-Nitrate Batteries.

Nitrate electroreduction reaction (eNO3 -RR) to ammonia (NH3) provides a promising strategy for nitrogen utilization, while achieving high selectivity and durability at an industrial scale has remained challenging. Herein, we demonstrated that the performance of eNO3 -RR could be significantly boosted by introducing two-dimensional Cu plates as electrocatalysts and eliminating the general carrier gas to construct a steady fluid field. The developed eNO3 -RR setup provided superior NH3 Faradaic efficiency (FE) of 99 %, exceptional long-term electrolysis for 120 h at 200 mA cm-2, and a record-high yield rate of 3.14 mmol cm-2 h-1. Furthermore, the proposed strategy was successfully extended to the Zn-nitrate battery system, providing a power density of 12.09 mW cm-2 and NH3 FE of 85.4 %, outperforming the state-of-the-art eNO3 -RR catalysts. Coupled with the COMSOL multiphysics simulations and in situ infrared spectroscopy, the main contributor for the high-efficiency NH3 production could be the steady fluid field to timely rejuvenate the electrocatalyst surface during the electrocatalysis.

Nitrogen Plasma Activates CoMn-Layered Double Hydroxides for Superior Electrochemical Oxygen Evolution.

Bimetallic layered double hydroxide is considered an ideal electrocatalytic material. However, due to the poor electrical conductivity of the bimetallic layered structure, obtaining highly active and stable catalysts through facile regulation strategies remains a great challenge. Herein, we use a simple corrosion strategy and nitrogen plasma technology to convert cobalt-based metal-organic frameworks into nitrogen-doped CoMn bimetallic layered double hydroxides (CoMn-LDH). Under the condition of regulating the local coordination environment of the catalytic active site and the presence of rich oxygen vacancy defects, N@CoMn-LDH/CC generates a low overpotential of 219 mV at 10 mA cm-2, which exceeds that of the commercial RuO2 catalyst. Density functional theory calculation shows that nitrogen doping improves the adsorption energy of the Mn site for oxygen evolution intermediates and reduces the reaction energy barrier of the Co site. Meanwhile, experiments and theoretical calculations verify that the mechanism of nitrogen doping regulating the oxygen evolution reaction (OER) follows the lattice oxygen oxidation mechanism, avoiding the collapse of the structure caused by catalyst reconstruction, thus improving the stability of oxygen evolution. This work provides a new simple strategy for the preparation of catalysts for a superior electrocatalytic oxygen evolution reaction.

Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H2 Production.

Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1 -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of -60 mV and overpotential of 32 mV for a current density of 10 mA cm-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall hydrazine splitting (OHzS) demonstrates outstanding activity with a record-high current density of 522 mA cm-2 at cell voltage of 0.3 V. DFT calculations elucidate the cooperative Ni(Co)-Ru-P sites in Ru1 -NiCoP optimize H* adsorption, and enhance adsorption of *N2 H2 to significantly lower the energy barrier for hydrazine dehydrogenation. Moreover, a self-powered H2 production system utilizing OHzS device driven by direct hydrazine fuel cell (DHzFC) achieve a satisfactory rate of 24.0 mol h-1 m-2 .

High Pseudocapacitance-Driven CoC2 O4 Electrodes Exhibiting Superior Electrochemical Kinetics and Reversible Capacities for Lithium-Ion and Lithium-Sulfur Batteries.

In this study, cuboid-like anhydrous CoC2 O4 particles (CoC2 O4 -HK) are synthesized through a potassium citrate-assisted hydrothermal method, which possess well-crystallized structure for fast Li+ transportation and efficient Li+ intercalation pseudocapacitive behaviors. When being used in lithium-ion batteries, the as-prepared CoC2 O4 -HK delivers a high reversible capacity (≈1360 mAh g-1 at 0.1 A g-1 ), good rate capability (≈650 mAh g-1 at 5 A g-1 ) and outstanding cycling stability (835 mAh g-1 after 1000 cycles at 1 A g-1 ). Characterizations illustrate that the Li+ -intercalation pseudocapacitance dominates the charge storage of CoC2 O4 -HK electrode, together with the reversible reaction of CoC2 O4 +2Li+ +2e- →Co+Li2 C2 O4 on discharging and charging. In addition, CoC2 O4 -HK particles are also used together with carbon-sulfur composite materials as the electrocatalysts for lithium-sulfur (Li-S) battery, which displays a gratifying sulfur electrochemistry with a high reversibility of 1021.5 mAh g-1 at 2 C and a low decay rate of 0.079% per cycle after 500 cycles. The density functional theory (DFT) calculations show that CoC2 O4 /C can regulate the adsorption-activation of reaction intermediates and therefore boost the catalytic conversion of polysulfides. Therefore, this work presents a new prospect of applying CoC2 O4 as the high-performance electrode materials for rechargeable Li-ion and Li-S batteries.

Zn0.52 V2 O5-a ⋠1.8 H2 O Cathode Stabilized by In Situ Phase Transformation for Aqueous Zinc-Ion Batteries with Ultra-Long Cyclability.

Developing cathode materials integrating good rate performance and sufficient cycle life is the key to commercialization of aqueous zinc-ion batteries. The hyperstable Zn0.52 V2 O5-a ⋅1.8 H2 O (ZVOH) cathode with excellent rate performance has been successfully developed via an in situ self-transformation from zinc-rich Zn3 V3 O8 (ZVO) in this study. Different from the common synthetic method of additional Zn2+ pre-insertion, ZVOH is obtained from the insertion of structural H2 O and the removal of excess Zn2+ in ZVO, ensuring the lattice structure of ZVOH remains relatively intact during the phase transition and rendering good structural stabilities. The ZVOH delivers a reversible capacity of 286.2 mAh g-1 at 0.2 A g-1 and of 161.5 mAh g-1 at 20 A g-1 over 18 000 cycles with a retention of 95.4 %, demonstrating excellent rate performance and cyclic stability. We also provide new insights on the structural self-optimization of Znx (CF3 SO3 )y (OH)2x-y ⋅n H2 O byproducts and the effect on the mobility of Zn2+ by theoretical calculations and experimental evidence.

Hydroxylated Multi-Walled Carbon Nanotubes Covalently Modified with Tris(hydroxypropyl) Phosphine as a Functional Interlayer for Advanced Lithium-Sulfur Batteries.

We have successfully constructed a new type of intercalation membrane material by covalently grafting organic tris(hydroxypropyl)phosphine (THPP) molecules onto hydroxylated multi-walled carbon nanotubes (CNT-OH) as a functional interlayer for the advanced LSBs. The as-assembled interlayer has been demonstrated to be responsible for the fast conversion kinetics of polysulfides, the inhibition of polysulfide shuttle effect, as well as the formation of a stable solid electrolyte interphase(SEI) layer. By means of spectroscopic and electrochemical analysis, we further found THPP plays a key role in accelerating the conversion of polysulfides into low-ordered lithium sulfides and suppressing the loss of polysulfides, thus rendering the as-designed lithium-sulfur battery in this work a high capacity, excellent rate performance and long-term stability. Even at low temperatures, the capacity decay rate was only 0.036 % per cycle for 1700 cycles.

Microenvironment Engineering for the Electrocatalytic CO2 Reduction Reaction.

Rather than just focusing on the catalyst itself in the electrocatalytic CO2 reduction reaction (eCO2 RR), as previously reviewed elsewhere, we herein extend the discussion to the special topic of the microenvironment around the electrocatalytic center and present a comprehensive overview of recent research progress. We categorize the microenvironment based on the components relevant to electrocatalytic active sites, i.e., the catalyst surface, substrate, co-reactants, electrolyte, membrane, and reactor. Supported by most of the reported articles, the relevant factors affecting the catalytic performance of eCO2 RR are then discussed in detail, and existing challenges and potential solutions are mentioned. Perspectives for the future research on eCO2 RR, including the integration of different microenvironment factors, the extension to industrial application by coupling with carbon capture and conversion, and separation of products, are also discussed.

Tailoring Hierarchically Porous Nitrogen-, Sulfur-Codoped Carbon for High-Performance Supercapacitors and Oxygen Reduction.

Heteroatom-doped carbon materials are intensively studied in supercapacitors and fuel cells, because of their great potential for sustainably bearing on the energy crisis and environmental pollution. Although enormous efforts are put in material perfection with a hierarchically porous microstructure, the simultaneous optimization of both porous structures and surface functionalities is hard to achieve due to inevitable concurrent dopant leaching effect and structural collapse under required high pyrolysis temperature. In this study, an in situ dehalogenation polymerization and activation protocol is introduced to synthesize nitrogen- and sulfur-codoped carbon materials (NS-PCMs) with hierarchical pore distribution and abundant surface doping, which endows them with good conductivity, abundant accessible active sites, and efficient mass transport. As a result, the as-prepared carbon materials (NS-a-PCM-1000) show an excellent mass specific capacitance of 461.5 F g-1 at a current density of 0.1 A g-1 , long cycle life (>23 k, 10 A g-1 ), and high device energy and power density (17.3 Wh kg-1 , 250 W kg-1 ). Significantly, NS-a-PCM-1000 also exhibits one of the highest oxygen reduction reaction activities (onset potential of 1.0 V vs reversible hydrogen electrode) in alkaline media among all reported metal-free catalysts.

Rapid and Controllable Synthesis of Nanocrystallized Nickel-Cobalt Boride Electrode Materials via a Mircoimpinging Stream Reaction for High Performance Supercapacitors.

Nickel-cobalt borides (denoted as NCBs) have been considered as a promising candidate for aqueous supercapacitors due to their high capacitive performances. However, most reported NCBs are amorphous that results in slow electron transfer and even structure collapse during cycling. In this work, a nanocrystallized NCBs-based supercapacitor is successfully designed via a facile and practical microimpinging stream reactor (MISR) technique, composed of a nanocrystallized NCB core to facilitate the charge transfer, and a tightly contacted Ni-Co borates/metaborates (NCBi ) shell which is helpful for OH- adsorption. These merits endow NCB@NCBi a large specific capacity of 966 C g-1 (capacitance of 2415 F g-1 ) at 1 A g-1 and good rate capability (633.2 C g-1 at 30 A g-1 ), as well as a very high energy density of 74.3 Wh kg-1 in an asymmetric supercapacitor device. More interestingly, it is found that a gradual in situ conversion of core NCBs to nanocrystallized Ni-Co (oxy)-hydroxides inwardly takes place during the cycles, which continuously offers large specific capacity due to more electron transfer in the redox reaction processes. Meanwhile, the electron deficient state of boron in metal-borates shells can make it easier to accept electrons and thus promote ionic conduction.

Mild-Temperature Solution-Assisted Encapsulation of Phosphorus into ZIF-8 Derived Porous Carbon as Lithium-Ion Battery Anode.

The high theoretical capacity of red phosphorus (RP) makes it a promising anode material for lithium-ion batteries. However, the large volume change of RP during charging/discharging imposes an adverse effect on the cyclability and the rate performance suffers from its low conductivity. Herein, a facile solution-based strategy is exploited to incorporate phosphorus into the pores of zeolitic imidazole framework (ZIF-8) derived carbon hosts under a mild temperature. With this method, the blocky RP is etched into the form of polyphosphides anions (PP, mainly P5 - ) so that it can easily diffuse into the pores of porous carbon hosts. Especially, the indelible crystalline surface phosphorus can be effectively avoided, which usually generates in the conventional vapor-condensation encapsulation method. Moreover, highly-conductive ZIF-8 derived carbon hosts with any pore smaller than 3 nm are efficient for loading PP and these pores can alleviate the volume change well. Finally, the composite of phosphorus encapsulated into ZIF-8 derived porous carbon exhibits a significantly improved electrochemical performance as lithium-ion battery anode with a high capacity of 786 mAh g-1 after 100 cycles at 0.1 A g-1 , a good stability within 700 cycles at 1 A g-1 , and an excellent rate performance.

The charge carrier dynamics, efficiency and stability of two-dimensional material-based perovskite solar cells.

Perovskites have been firmly established as one of the most promising materials for third-generation solar cells. There remain several great and lingering challenges to be addressed regarding device efficiency and stability. The photovoltaic efficiency of perovskite solar cells (PSCs) depends drastically on the charge-carrier dynamics. This complex process includes charge-carrier generation, extraction, transport and collection, each of which needs to be modulated in a favorable manner to achieve high performance. Two-dimensional materials (TDMs) including graphene and its derivatives, transition metal dichalcogenides (e.g., MoS2, WS2), black phosphorus (BP), metal nanosheets and two-dimensional (2D) perovskite active layers have attracted much attention for application in perovskite solar cells due to their high carrier mobility and tunable work function properties which greatly impact the charge carrier dynamics of PSCs. To date, significant advances have been achieved in the field of TDM-based PSCs. In this review, the recent progress in the development and application of TDMs (i.e., graphene, graphdiyne, transition metal dichalcogenides, BP, and others) as electrodes, hole transporting layers, electron transporting layers and buffer layers in PSCs is detailed. 2D perovskites as active absorber materials in PSCs are also summarized. The effect of TDMs and 2D perovskites on the charge carrier dynamics of PSCs is discussed to provide a comprehensive understanding of their optoelectronic processes. The challenges facing the PSC devices are emphasized with corresponding solutions to these problems provided with the overall goal of improving the efficiency and stability of photovoltaic devices.

Interfacially Bridging Covalent Network Yields Hyperstable and Ultralong Virus-Based Fibers for Engineering Functional Materials.

We present a strategy of interfacially bridging covalent network within tobacco mosaic virus (TMV) virus-like particles (VLPs). We arranged T103C cysteine to laterally conjugate adjacent subunits. In the axis direction, we set A74C mutation and systematically investigated candidate from E50C to P54C as the other thiol function site, for forming longitudinal disulfide bond chains. Significantly, the T103C-TMV-E50C-A74C shows the highest robustness in assembly capability and structural stability with the largest length, for TMV VLP to date. The fibers with lengths from several to a dozen of micrometers even survive under pH 13. The robust nature of this TMV VLP allows for reducer-free synthesis of excellent electrocatalysts for application in harshly alkaline hydrogen evolution.

Radially Inwardly Aligned Hierarchical Porous Carbon for Ultra-Long-Life Lithium-Sulfur Batteries.

Rational design of hollow micro- and/or nano-structured cathodes as sulfur hosts has potential for high-performance lithium-sulfur batteries. However, their further commercial application is hindered because infusing sulfur into hollow hosts is hard to control and the interactions between high loading sulfur and electrolyte are poor. Herein, we designed hierarchical porous hollow carbon nanospheres with radially inwardly aligned supporting ribs to mitigate these problems. Such a structure could aid the sulfur infusion and maximize sulfur utilization owing to the well-ordered pore channels. This highly organized internal carbon skeleton can also enhance the electronic conductivity. The hollow carbon nanospheres with further nitrogen-doping as the sulfur host material exhibit good capacity and excellent cycling performance (0.044 % capacity degradation per each cycle for 1000 cycles).