Synergistic regulation of hierarchical nanostructures and defect engineering is effective in accelerating electron and ion transport for metal oxide electrodes. Herein, carbon nanofiber-supported V2O3 with enriched oxygen vacancies (OV-V2O3@CNF) was fabricated using the facile electrospinning method, followed by thermal reduction. Differing from the traditional particles embedded within carbon nanofibers or irregularly distributed between carbon nanofibers, the free-standing OV-V2O3@CNF allows for V2O3 nanosheets to grow vertically on one-dimensional (1D) carbon nanofibers, enabling abundant active sites, shortened ion diffusion pathway, continuous electron transport, and robust structural stability. Meanwhile, density functional theory calculations confirmed that the oxygen vacancies can promote intrinsic electron conductivity and reduce ion diffusion energy barrier. Consequently, the OV-V2O3@CNF anode delivers a large reversible capacity of 812 mAh g–1 at 0.1 A g–1, superior rate capability (405 mAh g–1 at 5 A g–1), and long cycle life (378 mAh g–1 at 5 A g–1 after 1000 cycles). Moreover, an all-vanadium full battery (V2O5//OV-V2O3@CNF) was assembled using an OV-V2O3@CNF anode and a V2O5 cathode, which outputs a working voltage of 2.5 V with high energy density and power density, suggesting promising practical application. This work offers fresh perspectives on constructing hierarchical 1D nanofiber electrodes by combining defect engineering and electrospinning technology.
Most advanced hydrogen evolution reaction (HER) catalysts show high activity under alkaline conditions. However, the performance deteriorates at a natural and acidic pH, which is often problematic in practical applications. Herein, a rhenium (Re) sulfide–transition-metal dichalcogenide heterojunction catalyst with Re-rich vacancies (NiS2-ReS2-V) has been constructed. The optimized catalyst shows extraordinary electrocatalytic HER performance over a wide range of pH, with ultralow overpotentials of 42, 85, and 122 mV under alkaline, acidic, and neutral conditions, respectively. Moreover, the two-electrode system with NiS2-ReS2-V1 as the cathode provides a voltage of 1.73 V at 500 mA cm–2, superior to industrial systems. Besides, the open-circuit voltage of a single Zn–H2O cell with NiS2-ReS2-V1 as the cathode can reach an impressive 90.9% of the theoretical value, with a maximum power density of up to 31.6 mW cm–2. Moreover, it shows remarkable stability, with sustained discharge for approximately 120 h at 10 mA cm–2, significantly outperforming commercial Pt/C catalysts under the same conditions in all aspects. A series of systematic characterizations and theoretical calculations demonstrate that Re vacancies on the heterojunction interface would generate a stronger built-in electric field, which profoundly affects surface charge distribution and subsequently enhances HER performance.
Rational design and construction of oxygen reduction reaction (ORR) electrocatalysts with high activity, good stability, and low price are essential for the practical applications of renewable energy conversion devices, such as metal-air batteries. Electronic modification through constructing metal/semiconductor Schottky heterointerface represents a powerful strategy to enhance the electrochemical performance. Herein, we demonstrate a concept of Schottky electrocatalyst composed of uniform Co nanoparticles in situ anchored on the carbon nanotubes aligned on the carbon nanosheets (denoted as Co@N-CNTs/NSs hereafter) toward ORR. Both experimental findings and theoretical simulation testify that the rectifying contact could impel the voluntary electron flow from Co to N-CNTs/NSs and create an internal electric field, thereby boosting the electron transfer rate and improving the intrinsic activity. As a consequence, the Co@N-CNTs/NSs deliver outstanding ORR activity, impressive long-term durability, excellent methanol tolerance, and good performance as the air-cathode in the Zn-air batteries. The design concept of Schottky contact may provide the innovational inspirations for the synthesis of advanced catalysts in sustainable energy conversion fields.
The low ion transport is a major obstacle for low-temperature (LT) sodium-ion batteries (SIBs). Herein, a core-shell structure of bismuth (Bi) nanospheres coated with carbon (Bi@C) is constructed by utilizing a novel Bi-based complex (1,4,5,8-naphthalenetetracarboxylic dianhydride as the ligand) as the precursor, which provides an effective template to fabricate Bi-based anodes. At –40°C, the Bi@C anode achieves a high capacity, which is equivalent to 96% of that at 25°C, benefitting from the core-shell nanostructured engineering and Na+-ether-solvent cointercalation process. The special Na+-diglyme cointercalation behavior may effectively reduce the activation energy and accelerate the Na+ diffusion kinetics, enabling the excellent low-temperature performance of the Bi@C electrode. As expected, the fabricated Na3V2(PO4)3//Bi@C full-cell delivers impressive rechargeability in the ether-based electrolyte at –40°C. Density functional theory calculations and electrochemical tests also reveal the fast reaction kinetic mechanism at LT, thanks to a much lower diffusion energy barrier (167 meV) and a lower reaction activation energy (32.2 kJ mol–1) of Bi@C anode in comparison with that of bulk Bi. This work provides a rational design of Bi-based electrodes for rechargeable SIBs under extreme conditions.
Both sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs) are considered as promising candidates in grid-level energy storage devices. Unfortunately, the larger ionic radii of K+ and Na+ induce poor diffusion kinetics and cycling stability of carbon anode materials. Pore structure regulation is an ideal strategy to promote the diffusion kinetics and cyclic stability of carbon materials by facilitating electrolyte infiltration, increasing the transport channels, and alleviating the volume change. However, traditional pore-forming agent-assisted methods considerably increase the difficulty of synthesis and limit practical applications of porous carbon materials. Herein, porous carbon materials (Ca-PC/Na-PC/K-PC) with different pore structures have been prepared with gluconates as the precursors, and the amorphous structure, abundant micropores, and oxygen-doping active sites endow the Ca-PC anode with excellent potassium and sodium storage performance. For PIBs, the capacitive contribution ratio of Ca-PC is 82% at 5.0 mV s–1 due to the introduction of micropores and high oxygen-doping content, while a high reversible capacity of 121.4 mAh g–1 can be reached at 5 A g–1 after 2000 cycles. For SIBs, stable sodium storage capacity of 101.4 mAh g–1 can be achieved at 2 A g–1 after 8000 cycles with a very low decay rate of 0.65% for per cycle. This work may provide an avenue for the application of porous carbon materials in the energy storage field.
Rechargeable neutral aqueous zinc–air batteries (ZABs) are a promising type of energy storage device with longer operating life and less corrosiveness compared with conventional alkaline ZABs. However, the neutral ZABs normally possess poor oxygen evolution reactions (OERs) and oxygen reduction reactions performance, resulting in a large charge–discharge voltage gap and low round-trip efficiency. Herein, we demonstrate a sunlight-assisted strategy for achieving an ultralow voltage gap of 0.05 V in neutral ZABs by using the FeOOH-decorated BiVO4 (Fe-BiVO4) as an oxygen catalyst. Under sunlight, the electrons move from the valence band (VB) of Fe-BiVO4 to the conduction band producing holes in VB to promote the OER process and hence reduce the overpotential. Meanwhile, the photopotential generated by the Fe-BiVO4 compensates a part of the charging potential of neutral ZABs. Accordingly, the energy loss of the battery could be compensated via solar energy, leading to a record-low gap of 0.05 V between the charge and discharge voltage with a high round-trip efficiency of 94%. This work offers a simple but efficient pathway for solar-energy utilization in storage devices, further guiding the design of high energy efficiency of neutral aqueous ZABs.
Aqueous zinc-ion batteries have been regarded as the most potential candidate to substitute lithium-ion batteries. However, many serious challenges such as suppressing zinc dendrite growth and undesirable reactions, and achieving fully accepted mechanism also have not been solved. Herein, the commensal composite microspheres with α-MnO2 nano-wires and carbon nanotubes were achieved and could effectively suppress ZnSO4·3Zn(OH)2·nH2O rampant crystallization. The electrode assembled with the microspheres delivered a high initial capacity at a current density of 0.05 A g–1 and maintained a significantly prominent capacity retention of 88% over 2500 cycles. Furthermore, a novel energy-storage mechanism, in which multivalent manganese oxides play a synergistic effect, was comprehensively investigated by the quantitative and qualitative analysis for ZnSO4·3Zn(OH)2·nH2O. The capacity contribution of multivalent manganese oxides and the crystal structure dissection in the transformed processes were completely identified. Therefore, our research could provide a novel strategy for designing improved electrode structure and a comprehensive understanding of the energy storage mechanism of α-MnO2 cathodes.
Hard carbon is regarded as a promising anode candidate for sodium-ion batteries due to its low cost, relatively low working voltage, and satisfactory specific capacity. However, it still remains a challenge to obtain a high-performance hard carbon anode from cost-effective carbon sources. In addition, the solid electrolyte interphase (SEI) is subjected to continuous rupture during battery cycling, leading to fast capacity decay. Herein, a lignin-based hard carbon with robust SEI is developed to address these issues, effectively killing two birds with one stone. An innovative gas-phase removal-assisted aqueous washing strategy is developed to remove excessive sodium in the precursor to upcycle industrial lignin into high-value hard carbon, which demonstrated an ultrahigh sodium storage capacity of 359 mAh g–1. It is found that the residual sodium components from lignin on hard carbon act as active sites that controllably regulate the composition and morphology of SEI and guide homogeneous SEI growth by a near-shore aggregation mechanism to form thin, dense, and organic-rich SEI. Benefiting from these merits, the as-developed SEI shows fast Na+ transfer at the interphases and enhanced structural stability, thus preventing SEI rupture and reformation, and ultimately leading to a comprehensive improvement in sodium storage performance.
Due to the limitations of the raw materials and processes involved, polyolefin separators used in commercial lithium-ion batteries (LIBs) have gradually failed to meet the increasing requirements of high-end batteries in terms of energy density, power density, and safety. Hence, it is very important to develop next-generation separators for advanced lithium (Li)-based rechargeable batteries including LIBs and Li–S batteries. Nonwoven nanofiber membranes fabricated via electrospinning technology are highly attractive candidates for high-end separators due to their simple processes, low-cost equipment, controllable microporous structure, wide material applicability, and availability of multiple functions. In this review, the electrospinning technologies for separators are reviewed in terms of devices, process and environment, and polymer solution systems. Furthermore, strategies toward the improvement of electrospun separators in advanced LIBs and Li–S batteries are presented in terms of the compositions and the structure of nanofibers and separators. Finally, the challenges and prospects of electrospun separators in both academia and industry are proposed. We anticipate that these systematic discussions can provide information in terms of commercial applications of electrospun separators and offer new perspectives for the design of functional electrospun separators for advanced Li-based batteries.
The world’s population is growing, leading to an increasing demand for freshwater resources for drinking, sanitation, agriculture, and industry. Interfacial solar steam generation (ISSG) can solve many problems, such as mitigating the power crisis, minimizing water pollution, and improving the purification and desalination of seawater, rivers/lakes, and wastewater. Cellulosic materials are a viable and ecologically sound technique for capturing solar energy that is adaptable to a range of applications. This review paper aims to provide an overview of current advancements in the field of cellulose-based materials ISSG devices, specifically focusing on their applications in water purification and desalination. This paper examines the cellulose-based materials ISSG system and evaluates the effectiveness of various cellulosic materials, such as cellulose nanofibers derived from different sources, carbonized wood materials, and two-dimensional (2D) and 3D cellulosic-based materials from various sources, as well as advanced cellulosic materials, including bacterial cellulose and cellulose membranes obtained from agricultural and industrial cellulose wastes. The focus is on exploring the potential applications of these materials in ISSG devices for water desalination, purification, and treatment. The function, advantages, and disadvantages of cellulosic materials in the performance of ISSG devices were also deliberated throughout our discussion. In addition, the potential and suggested methods for enhancing the utilization of cellulose-based materials in the field of ISSG systems for water desalination, purification, and treatment were also emphasized.
This study explores a symmetric configuration approach in anion exchange membrane (AEM) water electrolysis, focusing on overcoming adaptability challenges in dynamic conditions. Here, a rapid and mild synthesis technique for fabricating fibrous membrane-type catalyst electrodes is developed. Our method leverages the contrasting oxidation states between the sulfur-doped NiFe(OH)2 shell and the metallic Ni core, as revealed by electron energy loss spectroscopy. Theoretical evaluations confirm that the S–NiFe(OH)2 active sites optimize free energy for alkaline water electrolysis intermediates. This technique bypasses traditional energy-intensive processes, achieving superior bifunctional activity beyond current benchmarks. The symmetric AEM water electrolyzer demonstrates a current density of 2 A cm–2 at 1.78 V at 60°C in 1 M KOH electrolyte and also sustains ampere-scale water electrolysis below 2.0 V for 140 h even in ambient conditions. These results highlight the system’s operational flexibility and structural stability, marking a significant advancement in AEM water electrolysis technology.
The dynamic surface self-reconstruction behavior in local structure correlates with oxygen evolution reaction (OER) performance, which has become an effective strategy for constructing the catalytic active phase. However, it remains a challenge to understand the mechanisms of reconstruction and to accomplish it fast and deeply. Here, we reported a photo-promoted rapid reconstruction (PRR) process on Ag nanoparticle-loaded amorphous Ni-Fe hydroxide nanosheets on carbon cloth for enhanced OER. The photogenerated holes generated by Ag in conjunction with the anodic potential contributed to a thorough reconstruction of the amorphous substrate. The valence state of unsaturated coordinated Fe atoms, which serve as active sites, is significantly increased, while the corresponding crystalline substrate shows little change. The different structural evolutions of amorphous and crystalline substrates during reconstruction lead to diverse pathways of OER. This PRR utilizing loaded noble metal nanoparticles can accelerate the generation of active species in the substrate and increase the electrical conductivity, which provides a new inspiration to develop efficient catalysts via reconstruction strategies.
For lithium-sulfur batteries (Li-S batteries), a high-content electrolyte typically can exacerbate the shuttle effect, while a lean electrolyte may lead to decreased Li-ion conductivity and reduced catalytic conversion efficiency, so achieving an appropriate electrolyte-to-sulfur ratio (E/S ratio) is essential for improving the battery cycling efficiency. A quasi-solid electrolyte (COF-SH@PVDF-HFP) with strong adsorption and high catalytic conversion was constructed for in situ covalent organic framework (COF) growth on highly polarized polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) fibers. COF-SH@PVDF-HFP enables efficient Li-ion conductivity with low-content liquid electrolyte and effectively suppresses the shuttle effect. The results based on in situ Fourier-transform infrared, in situ Raman, UV–Vis, X-ray photoelectron, and density functional theory calculations confirmed the high catalytic conversion of COF-SH layer containing sulfhydryl and imine groups for the lithium polysulfides. Lithium plating/stripping tests based on Li/COF-SH@PVDF-HFP/Li show excellent lithium compatibility (5 mAh cm–2 for 1400 h). The assembled Li-S battery exhibits excellent rate (2 C 688.7 mAh g–1) and cycle performance (at 2 C of 568.8 mAh g–1 with a capacity retention of 77.3% after 800 cycles). This is the first report to improve the cycling stability of quasi-solid-state Li-S batteries by reducing both the E/S ratio and the designing strategy of sulfhydryl-functionalized COF for quasi-solid electrolytes. This process opens up the possibility of the high performance of solid-state Li-S batteries.
Solar-driven interfacial evaporation is a promising technology for freshwater production from seawater, but salt accumulation on the evaporator surface hinders its performance and sustainability. In this study, we report a simple and green strategy to fabricate a three-dimensional porous graphene spiral roll (3GSR) that enables highly efficient solar evaporation, salt collection, and water production from near-saturated brine with zero liquid discharge (ZLD). The 3GSR design facilitates energy recovery, radial brine transport, and directional salt crystallization, thereby resulting in an ultrahigh evaporation rate of 9.05 kg m–2 h–1 in 25 wt% brine under 1-sun illumination for 48 h continuously. Remarkably, the directional salt crystallization on its outer surface not only enlarges the evaporation area but also achieves an ultrahigh salt collection rate of 2.92 kg m–2 h–1, thus enabling ZLD desalination. Additionally, 3GSR exhibits a record-high water production rate of 3.14 kg m–2 h–1 in an outdoor test. This innovative solution offers a highly efficient and continuous solar desalination method for water production and ZLD brine treatment, which has great implications for addressing global water scarcity and environmental issues arising from brine disposal.
High electrochemical stability and safety make Na+ superionic conductor (NASICON)-class cathodes highly desirable for Na-ion batteries (SIBs). However, their practical capacity is limited, leading to low specific energy. Furthermore, the low electrical conductivity combined with a decline in capacity upon prolonged cycling (>1000 cycles) related to the loss of active material-carbon conducting contact regions contributes to moderate rate performance and cycling stability. The need for high specific energy cathodes that meet practical electrochemical requirements has prompted a search for new materials. Herein, we introduce a new carbon-coated Na3VFe0.5Ti0.5(PO4)3 (NVFTP/C) material as a promising candidate in the NASICON family of cathodes for SIBs. With a high specific energy of ˜457 Wh kg–1 and a high Na+ insertion voltage of 3.0 V versus Na+/Na, this cathode can undergo a reversible single-phase solid-solution and two-phase (de)sodiation evolution at 28 C (1 C = 174.7 mAh g–1) for up to 10,000 cycles. This study highlights the potential of utilizing low-cost and highly efficient cathodes made from Earth-abundant and harmless materials (Fe and Ti) with enriched Na+-storage properties in practical SIBs.
Interfacial electronic structure modulation of nickel-based electrocatalysts is significant in boosting energy-conversion-relevant urea oxidation reaction (UOR). Herein, porous carbon nanofibers confined mixed Ni-based crystal phases of Ni2P and NiF2 are developed via fluorination and phosphorization of Ni coated carbon nanofiber (Ni2P/NiF2/PCNF), which possess sufficient mesoporous and optimized Gibbs adsorption free energy by mixed phase-induced charge redistribution. This novel system further reduces the reaction energy barrier and improves the reaction activity by addressing the challenges of low intrinsic activity, difficulty in active site formation, and insufficient synergism. A considerably high current density of 254.29 mA cm–2 is reached at 1.54 V versus reversible hydrogen electrode on a glass carbon electrode, and the cell voltage requires 1.39 V to get 10 mA cm–2 in hydrogen generation, with very good stability, about 190 mV less than that of the traditional water electrolysis. The facile active phase formation and high charge transfer ability induced by asymmetric charge redistribution are found in the interface, where the urea molecules tend to bond with Ni atoms on the surface of heterojunction, and the rate-determining step is changed from CO2 desorption to the fourth H-atom deprotonation. The work reveals a novel catalyst system by interfacial charge redistribution induced by high bond polarity for energy-relevant catalysis reactions.
Designing high-performance and low-cost electrocatalysts for oxygen evolution reaction (OER) is critical for the conversion and storage of sustainable energy technologies. Inspired by the biomineralization process, we utilized the phosphorylation sites of collagen molecules to combine with cobalt-based mononuclear precursors at the molecular level and built a three-dimensional (3D) porous hierarchical material through a bottom-up biomimetic self-assembly strategy to obtain single-atom catalysts confined on carbonized biomimetic self-assembled carriers (Co SACs/cBSC) after subsequent high-temperature annealing. In this strategy, the biomolecule improved the anchoring efficiency of the metal precursor through precise functional groups; meanwhile, the binding-then-assembling strategy also effectively suppressed the nonspecific adsorption of metal ions, ultimately preventing atomic agglomeration and achieving strong electronic metal-support interactions (EMSIs). Experimental characterizations confirm that binding forms between cobalt metal and carbonized self-assembled substrate (Co–O4–P). Theoretical calculations disclose that the local environment changes significantly tailored the Co d-band center, and optimized the binding energy of oxygenated intermediates and the energy barrier of oxygen release. As a result, the obtained Co SACs/cBSC catalyst can achieve remarkable OER activity and 24 h durability in 1 M KOH (η10 at 288 mV; Tafel slope of 44 mV dec–1), better than other transition metal-based catalysts and commercial IrO2. Overall, we presented a self-assembly strategy to prepare transition metal SACs with strong EMSIs, providing a new avenue for the preparation of efficient catalysts with fine atomic structures.
Rational design of efficient pH-universal hydrogen evolution reaction catalysts to enable large-scale hydrogen production via electrochemical water splitting is of great significance, yet a challenging task. Herein, Ru atoms in the Ru2P structure were replaced with M = Co, Ni, or Mo to produce M2–xRuxP nanocrystals. The metals show strong site preference, with Co and Ni occupying the tetrahedral sites and Ru the square pyramidal sites of the CoRuP and NiRuP Ru2P-type structures. The presence of Co or Ni in the tetrahedral sites leads to charge redistribution for Ru and, according to density functional theory calculations, a significant increase in the Ru d-band centers. As a result, the intrinsic activity of CoRuP and NiRuP increases considerably compared to Ru2P in both acidic and alkaline media. The effect is not observed for MoRuP, in which Mo prefers to occupy the pyramidal sites. In particular, CoRuP shows state-of-the-art activity, outperforming Ru2P with Pt-like activity in 0.5 M H2SO4 (η10 = 12.3 mV; η100 = 52 mV; turnover frequency (TOF) = 4.7 s–1). It remains extraordinarily active in alkaline conditions (η10 = 12.9 mV; η100 = 43.5 mV) with a TOF of 4.5 s–1, which is 4x higher than that of Ru2P and 10x that of Pt/C. Further increase in the Co content does not lead to drastic loss of activity, especially in alkaline medium, where, for example, the TOF of Co1.9Ru0.1P remains comparable to that of Ru2P and higher than that of Pt/C, highlighting the viability of the adopted approach to prepare cost-efficient catalysts.
Potassium-ion batteries (PIBs) offer a cost-effective and resource-abundant solution for large-scale energy storage. However, the progress of PIBs is impeded by the lack of high-capacity, long-life, and fast-kinetics anode electrode materials. Here, we propose a dual synergic optimization strategy to enhance the K+ storage stability and reaction kinetics of Bi2S3 through two-dimensional compositing and cation doping. Externally, Bi2S3 nanoparticles are loaded onto the surface of three-dimensional interconnected Ti3C2Tx nanosheets to stabilize the electrode structure. Internally, Cu2+ doping acts as active sites to accelerate K+ storage kinetics. Various theoretical simulations and ex situ techniques are used to elucidate the external–internal dual synergism. During discharge, Ti3C2Tx and Cu2+ collaboratively facilitate K+ intercalation. Subsequently, Cu2+ doping primarily promotes the fracture of Bi2S3 bonds, facilitating a conversion reaction. Throughout cycling, the Ti3C2Tx composite structure and Cu2+ doping sustain functionality. The resulting Cu2+-doped Bi2S3 anchored on Ti3C2Tx (C-BT) shows excellent rate capability (600 mAh g–1 at 0.1 A g–1; 105 mAh g–1 at 5.0 A g–1) and cycling performance (91 mAh g–1 at 5.0 A g–1 after 1000 cycles) in half cells and a high energy density (179 Wh kg–1) in full cells.
Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 phase. However, their practical applications are seriously obstructed by difficulties in thermodynamic phase regulation, complicated electrochemical phase transition, and unsatisfactory cycling life. Herein, we propose an efficient structural evolution strategy from biphase to monophase of Na0.766+xLixNi0.33–xMn0.5Fe0.1Ti0.07O2 through Li+ substitution. The role of Li+ substitution not only simplifies the unfavorable phase transition by altering the local coordination of transition metal (TM) cations but also stabilizes the cathode–electrolyte interphase to prevent the degradation of TM cations during battery cycling. As a result, the thermodynamically robust O3-Na0.826Li0.06Ni0.27Mn0.5Fe0.1Ti0.07O2 cathode delivers a high capacity of 139.4 mAh g–1 at 0.1 C and shows prolonged cycling life at high rates, with capacity retention of 81.6% at 5 C over 500 cycles. This work establishes a solid relationship between the thermodynamic structure evolution and electrochemistry of layered cathode materials, contributing to the development of long-life sodium-ion batteries.
The buried interface in the perovskite solar cell (PSC) has been regarded as a breakthrough to boost the power conversion efficiency and stability. However, a comprehensive manipulation of the buried interface in terms of the transport layer, buried interlayer, and perovskite layer has been largely overlooked. Herein, we propose the use of a volatile heterocyclic compound called 2-thiopheneacetic acid (TPA) as a pre-buried additive in the buried interface to achieve cross-layer all-interface defect passivation through an in situ bottom-up infiltration diffusion strategy. TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film. Owing to this versatility, TPA-tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long-term stability. This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC.
Lithium metal shows a great advantage as the most promising anode for its unparalleled theoretical specific capacity and extremely low electrochemical potential. However, uncontrolled lithium dendrite growth and severe side reactions of the reactive intermediates and organic electrolytes still limit the broad application of lithium metal batteries. Herein, we propose 4-nitrobenzenesulfonyl fluoride (NBSF) as an electrolyte additive for forming a stable organic–inorganic hybrid solid electrolyte interphase (SEI) layer on the lithium surface. The abundance of lithium fluoride and lithium nitride can guarantee the SEI layer’s toughness and high ionic conductivity, achieving dendrite-free lithium deposition. Meanwhile, the phenyl group of NBSF significantly contributes to both the chemical stability of the SEI layer and the good adaptation to volume changes of the lithium anode. The lithium–oxygen batteries with NBSF exhibit prolonged cycle lives and excellent cycling stability. This simple approach is hoped to improve the development of the organic–inorganic SEI layer to stabilize the lithium anodes for lithium–oxygen batteries.