Interfacial Charge Research Articles

Dual LSPR and CT synergy: 3D urchin-like Au@W18O49 enables highly sensitive in-situ SERS detection of dissolved furfural in insulating oils

Assessing the levels of furfural in insulating oils is a crucial technical method for evaluating the degree of aging and mechanical deterioration of oil-paper insulation. The surface-enhanced Raman spectroscopy (SERS) technique provides an effective method for enhancing the sensitivity of in-situ detection of furfural. In this study, a homogeneous three-dimensional (3D) urchin-like Au@W18O49 heterostructure was synthesized as a SERS substrate using a straightforward hydrothermal method. The origin of the superior Raman enhancement properties of the 3D urchin-like heterostructures formed by the noble metal Au and the plasmonic semiconductor W18O49, which is rich in oxygen vacancies, is analyzed experimentally in conjunction with density-functional theory (DFT) calculations. The Raman enhancement is further amplified by the remarkable dual localized surface plasmon resonance (LSPR) effect, which generates a strong local electric field and creates numerous "hot spots," in addition to the interfacial charge transport (CT). The synergistic effect of these factors results in the 3D urchin-like Au@W18O49 heterostructure exhibiting exceptionally high SERS activity. Testing the rhodamine 6G (R6G) probe resulted in a Raman enhancement factor of 3.41 × 10−8, and the substrate demonstrated excellent homogeneity and stability. Furthermore, the substrate was effectively utilized to achieve highly sensitive in-situ surface-enhanced Raman scattering (SERS) detection of dissolved furfural in complex plant insulating oils. The development of the 3D urchin-like Au@W18O49 heterostructure and the exploration of its enhancement mechanism provide theoretical insights for the advancement of high-performance SERS substrates.

Efficient generation of singlet oxygen (1O2) by CoP/Ni2P@NF for degradation of sulfamerazine through a heterogeneous electro-Fenton process at circumneutral pH

In electro-Fenton (EF), the development of a catalytic material with wide pH application range and high interference resistance is more suitable for practical wastewater treatment. In this study, the nanoneedle-shaped CoP/Ni2P heterostructure loaded onto a nickel foam substrate (CoP/Ni2P@NF) was successfully fabricated, which was used as a cathode material for heterogeneous electro-Fenton (Hetero-EF) to degrade sulfamerazine (SMR) at circumneutral pH. The SMR degradation efficiency within 90 min went to 100% and 87% at initial pH of 6.8 and 11, respectively. Experiments and theoretical calculations demonstrated that the heterostructure of CoP/Ni2P redistributed the interfacial charge and accelerated the electron transfer, resulting in different two-electron oxygen reduction (2e−ORR) selectivity and activity than CoP and Ni2P. The ion interference and complex water quality experiment exhibited that the degradation performance remained almost unchanged, showing better anti-interference ability and complex water quality applications. Through quenching experiments and EPR tests, it is confirmed that singlet oxygen (1O2) was the major reactive oxygen species (ROS) and 1O2 was converted from hydroxyl radical (·OH) adsorbed on the catalyst surface. This study provides an efficient catalyst for the application of Hetero-EF to remove organic compounds in complex water at circumneutral pH.

Water-Based Recycling Process of FTO/SnO2 Substrate for Sustainable Perovskite Solar Cell Technology.

Fluorine-doped tin oxide (FTO) substrate is an important and expensive component in perovskite solar cells (PSCs), which accounts for up to 40% of a typical PSC raw material cost. In this study, we investigated the recyclability of SnO2/FTO in PSCs by washing the spent PSCs using different solvent such as dimethylformamide (DMF), dimethylsulfoxide (DMSO), acetone, water, and acetone/water mixture. Characterisation of properties of the SnO2/FTO substrates recovered from the PSCshow the surface wettability of SnO2/FTO is largely unchanged with water washing while a higher hydrophobicity is obtained with organic solvent washing. Comparison of electronic properties of the SnO2/FTO substrate shows a downward shift of the conduction band by 180 meV with water washing, creating favourable energy alignment with adjacent perovskite for efficient interfacial charge injection. Consequently, PSCs using the water-based recycled SnO2/FTO substrates produced a high power conversion efficiency (PCE) of 19.33% which is comparable to the device using fresh SnO2/FTO substrate (PCE = 19.85%). Furthermore, we demonstrated that the water washing process could retain property of SnO2/FTO substrate for decent PSC performance up to four recycling cycles. This study opens new avenues towards recycling of valuable FTO substrates in PSCs for increased sustainability and cost-effectiveness.

Minimizing voltage loss for perovskite solar cells via synergistically passivating defects and reinforcing interfacial electric field

Perovskite solar cells have attracted much attention because of their excellent photoelectric properties. However, non-radiative recombination losses due to interface defects limit the open circuit voltage (Voc) of PSCs, which prevents further improvement in power conversion efficiency (PCE). To solve this problem, we introduced Li2SO4 into the SnO2/perovskite interface to obtain a higher Voc through interfacial passivation and enhancement of the interface electric field. Herein, Li+ presents bottom-up diffusion into perovskite surface, and forms dipoles with FA to enhance the interface electric field. Furthermore, SO in SO42- passivates Sn4+ on the surface of SnO2 and Pb2+ at the buried interface of perovskite. This method combines interfacial passivation with synchronous electric field enhancement, which promotes interfacial carrier migration and reduces non-radiative recombination and voltage loss (Vloss) at the interface. As a result, the SLS-device exhibits an enhanced Voc of 1.25 V, with a very low Vloss of 0.33 V, achieving an outstanding PCE of 24.31 %. Moreover, the device maintained 90 % of the initial PCE after exposure to ambient air for 1000 h. This work demonstrates the necessity to co-design the interface microstructure and electric field distribution for reducing the energy loss of perovskite photovoltaic devices and promoting the efficiency of interfacial charge transport.

Heterovalent Samarium Cation‐Doped SnO2 Electron Transport Layer for High‐Efficiency Planar Perovskite Solar Cells

Tin oxide (SnO2) has demonstrated significant potential as an electron transport layer (ETL) owing to its low‐temperature processing in perovskite solar cells (PSCs). However, the poor energy‐level alignment and the presence of interface defects between the SnO2 and perovskite layer aggravate the power conversion efficiency (PCE) of the PSCs. Herein, heterovalent samarium cation (Sm3+) is deliberately doped into SnO2, optimizing the energy‐level alignment between SnO2 and the perovskite layer, and effectively passivating the oxygen vacancy defects on the surface of SnO2. Experimental and theoretical conclusions reveal that Sm‐doping successfully passivates the defects in the ETL and improves the perovskite crystal quality, thereby reducing interface charge recombination, and enhancing electron extraction from perovskite to the SnO2 layer. Consequently, the optimized Sm‐doped SnO2‐based PSCs achieve a PCE of 24.10% with a VOC of 1.174 V, negligible hysteresis, and improved durability under ambient conditions.

Efficient Charge Carriers Separation and Transfer Driven by Interface Electric Field in FeS2@ZnIn2S4 Heterojunction Boost Hydrogen Evolution.

Photocatalytic H2 evolution technology is regarded as a promising and green route for the urgent requirement of efficient H2 production. At present, low efficiency is a major bottleneck that limits the practical application of photocatalytic H2 evolution. The construction of high-activity photocatalysts is highly crucial for achieving advanced hydrogen generation. Herein, a new S-scheme FeS2@ZnIn2S4 (FeS2@ZIS) heterostructure as the photocatalyst was developed for enhanced photocatalytic H2 evolution. Density function theory (DFT) calculation results strongly demonstrated that FeS2@ZIS generates a giant interface electric field (IEF), thus promoting the separation efficiency of photogenerated charge carriers for efficient visible-light-driven hydrogen evolution. At optimal conditions, the H2 production rate of the 8%FeS2@ZIS is 5.3 and 3.6 times higher than that of the pure FeS2 and ZIS, respectively. The experimental results further indicate that the close contact between FeS2 and ZIS promotes the formation of the S-scheme heterojunction, where the interfacial charge transfer achieves spatial separation of charge carriers. This further broadens the light absorption range of the FeS2@ZIS and improves the utilization rate of photogenerated charge carriers. This work thus offers new insights that the FeS2-based co-catalyst can enrich the research on S-scheme heterojunction photocatalysts and improve the transfer and separation efficiency of photogenerated carriers for photocatalytic hydrogen production.

Heterogeneous NASICON-Type Cathode With Reversible Multielectron Reaction for High-Performance Sodium-Ion Batteries.

Na superionic conductor (NASICON)-structured compounds demonstrate great application potential by their robust framework and compositional diversity. However, they are blamed for the mediocre energy density, and achieving both multielectron reaction and good cycling stability simultaneously is challenging. Herein, a novel heterogeneous Na4Fe3(PO4)2(P2O7)/Na2VTi(PO4)3 (NFPP/NVTP) material with stable multielectron reaction is constructed by spray drying technology. The mutual promotion effect of intergrowth structures effectively improves the purity and the crystallization of NFPP/NVTP during the fabrication process, which is beneficial to the high capacity and cycling stability. As a result, the optimized NFPP/NVTP demonstrates a high reversible capacity of 155.3 mAh g-1 at 20mA g-1 and outstanding cycling stability with 82.9% capacity retention over 2500 cycles at 1 A g-1, which are much superior to those of NFPP and NVTP individually. Even in full cell configuration, the energy density remains high at ≈380Wh kg-1 based on the cathode mass. The high capacity of NFPP/NVTP is also attributed to the successive reduction/oxidation mechanism involving the introduction of Ti3+ and interfacial charge redistribution effect between the heterogeneous phases, which greatly improve the electronic and ionic conductivity. Moreover, high reversible structural evolution during the multisodium storage process further guarantees excellent cycling stability.

Uniform nanorhombic α-Fe2O3 on g-C3N4 nanosheet: 2D/2D lattice matched S-scheme heterojunction towards efficient styrene oxidation and H2 evolution

The design and modification of heterojunction photocatalysts to enhance efficient interfacial charge transfer and superior photocatalytic performance are fundamental objectives in the field of solar-light-driven energy conversion and production. This study presents a novel S-scheme heterojunction which features lattice-matched morphological hetero-nanostructures, composing of two-dimensional (2D) graphitic carbon nitride (CN) loaded with uniformly distributed and size-consistent 2D nano-rhombohedral α-Fe2O3 (Fe2O3 NR/CN). The directional charge transfer in the lattice-matched S-scheme heterojunction was confirmed using a combination of in situ irradiated X-ray photoelectron spectroscopy, metal deposition experiments, electron paramagnetic resonance, and density functional theory calculations. The optimized heterojunction demonstrates exceptional photocatalytic activity, achieving a hydrogen generation rate that surpasses those of g-C3N4 and α-Fe2O3 alone by factors of 2.1 and 7, respectively. Additionally, this heterojunction exhibits an excellent styrene conversion rate of 94.1 % and a styrene epoxidation selectivity of 95.3 % under light irradiation at 80 °C using tert-butyl hydroperoxide (TBHP) as the oxidant. The incorporation of uniformly distributed nano-rhombohedral α-Fe2O3 particles with g-C3N4 successfully constructs an unobstructed interfacial pathway to form the lattice-matched S-scheme heterojunction, enabling efficient separation of photogenerated carriers. This unique structure provides a valuable reference for dual-functional photocatalytic reactions.

N-doped carbon dots-modulated interfacial charge transfer and surface structure in FeNbO4 photocatalysts for enhanced CO2 conversion selectivity to CH4

The photocatalytic carbon dioxide reduction reaction (CO2RR) is an innovative and reliable technology to address the issues of energy shortage and climate change simultaneously. However, issues such as insufficient light absorption, rapid electron-hole recombination and low surface activity during CO2RR severely limit the catalysts’ efficiency for photocatalysis. In this study, we present nanohybrid N-CDs/FeNbO4 catalysts to overcome these challenges and achieve high-efficient photocatalytic conversion of CO2 to CH4. The enhancement process starts with the introduction of modified N-CDs, which have a broad light absorption capability. These N-CDs also help to modulate the interfacial charge transfer kinetics, leading to improved charge separation and transfer. This, in turn, enhances the multielectron transfer conversion selectivity of CO2 to CH4. Meanwhile, CO2 adsorption on the photocatalysts is increased due to the creation of oxygen vacancies and lattice stresses resulting from the introduction of N-CDs. This work presents a new approach for improving the photocatalytic performance by adjusting surface structure and interfacial behaviors.

Exploring electrochemical kinetic behaviors and interfacial charge transfer of pure and Ni-doped ZnFe2O4 nanoparticles-based sensing nanoplatform for ultra-sensitive detection of chloramphenicol

ZnFe2O4 (ZFO) nanomaterial was doped with a divalent transition metal cation of Ni2+ (NixZn1-xFe2O4, x=0, 0.2, 0.4, and 0.8) and characterized by various analytical techniques. Powder X-ray diffraction revealed the formation of a single-phase cubic spinel structure, while the stabilization of crystal structure for Ni2+-doped samples was observed. The average crystalline size, d-spacing, and lattice parameters increased with increasing in Ni2+ concentration within NixZn1-xFe2O4, due to differences in the ionic radius, the cation distribution at A-B sites, and the creation of surface oxygen vacancies within ZFO structure. From electrochemical measurements, NixZn1-xFe2O4-based electrodes showed excellent enhancements in charge transfer ability and conductivity with the highest rate constant (0.018 ms−1), the lowest peak-to-peak separation (206 mV), the lowest Rct (118 Ω), and the largest electrochemical active area (0.248 cm2), compared to that of bare SPE. Among them, Ni0.8Zn0.2Fe2O4/SPE provided outstanding electrochemical behaviors and achieved the best sensing performance with the widened concentration linear range from 0.25 to 50 μM and a rather low detection limit of 0.2 μM for chloramphenicol detection. The most important reason for this positive advance comes from the unique synergistic effects of Ni doping into the ZFO host structure. The excellent enhancements in adsorption capacity (Г) (1.4 times higher), number of oxygen vacancies, charge transfer rate constant (approximately 1.15 times higher), and catalytic rate constant (30 times greater) were recorded at Ni-doped ZFO-based electrodes, compared to pure ZFO-based electrode. Furthermore, the detailed hypotheses and possible mechanisms explaining these impressive enhancements were explored. Our work provides insight into the correlation between the Ni-doping and electrochemical characteristics, which has implications for tailoring the electrochemical performance of spinel ferrites across diverse applications and the design of novel spinel ferrite nanomaterials.

High-performance hydrogen sensor based on γ-Fe2O3/α-Fe2O3 heterostructures produced by a one-step hydrothermal method

The construction of heterostructures is an effective strategy for enhancing the properties of functional materials. However, the problem of the weak built-in field at the heterointerface usually degrades the interfacial charge transfer efficiency, severely limiting the improvement of the sensing properties of gas sensors. To overcome this limitation, γ-Fe2O3/α-Fe2O3 (p-p) heterojunction structures were constructed via a one-step hydrothermal method. Interestingly, the morphology and structure of the Fe2O3 nanocrystals could be easily controlled by the amount of urea (CH4N2O). Thus, the response of Fe2O3-M to H2 (200 ppm) at 280 °C was 2.2 and 1.2 times greater than that of Fe2O3–R and Fe2O3–N, respectively. In addition, density functional theory (DFT) calculations were used to explore the sensing mechanism in detail, further confirming the experimental conclusions. The strong and ultrafast response to hydrogen was attributed to the synergistic effects of the unique heterostructure and large specific surface area. The development of efficient and stable new hydrogen-sensing materials will help further expand their application scope in the sensing field.

Improved UV Photoresponse Performance of ZnO Nanowire Array Photodetector via Effective Pt Nanoparticle Coupling.

Ultraviolet (UV) photodetectors (PDs) based on nanowire (NW) hold significant promise for applications in fire detection, optical communication, and environmental monitoring. As optoelectronic devices evolve towards lower dimensionality, multifunctionality, and integrability, multicolor PDs have become a research hotspot in optics and electronic information. This study investigates the enhancement of detection capability in a light-trapping ZnO NW array through modification with Pt nanoparticles (NPs) via magnetron sputtering and hydrothermal synthesis. The optimized PD exhibits superior performance, achieving a responsivity of 12.49 A/W, detectivity of 4.07 × 1012 Jones, and external quantum efficiency (EQE) of 4.19 × 103%, respectively. In addition, the Pt NPs/ZnO NW/ZnO PD maintains spectral selectivity in the UV region. These findings show the pivotal role of Pt NPs in enhancing photodetection performance through their strong light absorption and scattering properties. This improvement is associated with localized surface plasmon resonance induced by the Pt NPs, leading to enhanced incident light and interfacial charge separation for the specialized configurations of the nanodevice. Utilizing metal NPs for device modification represents a breakthrough that positively affects the preparation of high-performance ZnO-based UV PDs.

Designing TiO2 Nanotubular Arrays with Au-CoOx Core-Shell Nanoparticles for Enhanced Photoelectrochemical Methanol and Lignin Oxidation.

One-dimensional (1D) ordered TiO2 nanotubes exhibit exceptional charge transfer capabilities, making them suitable candidates for constructing visible-light-active photoanodes in selective PEC oxidation reactions. Herein, we employed a facile and easily scalable electrochemical method to fabricate Au-CoOx-deposited ordered TiO2 nanotubular array photoanodes. The improved visible light absorption capacity of TiO2-Au-CoOx, with unhampered 1D channels and the controlled integration of Au between TiO2 and CoOx, along with their synergistic interaction, have been identified as the most promising strategy for enhanced PEC performance, as evidenced by an IPCE of 3.7% at 450 nm. Furthermore, the robust interfacial charge transfer pathway from CoOx to the TiO2 surface via the Au mediator promotes the migration of photogenerated electrons and enables the accumulation of holes on the surface of CoOx. These holes are then efficiently utilized by oxidants such as methanol or lignin to generate value-added products, highlighting the potential of this system for advanced PEC applications.

Electronic and Transport Engineering of A-Type Antiferromagnets with Ferroelectric Sandwich Structure: Toward Multistate Nonvolatile Memory Applications.

Achieving higher-order multistates with mutual interstate switching at the nanoscale is essential for high-density storage devices; yet, it remains a significant challenge. Here, we demonstrate that integrating A-type antiferromagnetic semiconductors sandwiched between ferroelectric layers is an effective strategy to achieve high-performance multistate data storage. Taking the Sc2CO2/VSi2P4 bilayer (bi-VSi2P4)/Sc2CO2 van der Waals multiferroic heterostructure as an example, our first-principles calculations show that by switching the polarization direction of the upper and bottom ferroelectric Sc2CO2 layers, antiferromagnetic bi-VSi2P4 can exhibit four distinct states with different band structures. The intriguing band structure engineering stems from the polarization-field-induced band shift and interface charge transfer. Accordingly, the proposed Sc2CO2/bi-VSi2P4/Sc2CO2-based multiferroic device can achieve four different resistance states, accompanied by fully spin-polarized currents and giant tunneling electroresistance ratios. Our results propose a viable strategy for realizing nonvolatile electrical control of antiferromagnets at the nanoscale and provide insights into the development of advanced memories.

Hydrogen Bonds and In situ Photoinduced Metallic Bi0/Ni0 Accelerating Z-Scheme Charge Transfer of BiOBr@NiFe-LDH for Highly Efficient Photocatalysis.

For heterojunction system, the lack of stable interfacial driving force and definite charge transfer channel makes the charge separation and transfer efficiency unsatisfactory. The photoreaction mechanism occurring at the interface also receives less attention. Herein, a 2D/2D Z-scheme junction BiOBr@NiFe-LDH with large-area contact featured by short interface hydrogen bonds and strong interfacial electric field (IEF) is synthesized, and in situ photoinduced metallic species assisting charge transfer mechanism is demonstrated. The hydrogen bonds between O atoms from BiOBr and H atoms from NiFe-LDH induce a significant interfacial charge redistribution, establishing a robust IEF. Notably, during photocatalytic reaction, Bi0 and Ni0 are in situ performed in heterojunction, which separately act as electron transport mediator and electron trap to further accelerate charge transfer efficiency up to 71.2 %. Theoretical calculations further demonstrate that the existence of Bi0 strengthens the IEF. Therefore, high-speed spatial charge separation is realized in Bi0/BiOBr@Ni0/NiFe-LDH, leading to a prominent photocatalytic activity with a tetracycline removal ratio of 88.3 % within 7 min under visible-light irradiation and the presence of persulfate, far exceeding majority of photocatalysts reported previously. This study provides valid insights for designing hydrogen bonding heterojunction systems, and advances mechanistic understanding on in situ photoreaction at interfaces.

Electronic interaction and band alignment between Cu sub-nanometric clusters and ZnIn2S4 nanosheets towards selective photoreduction of CO2 to CO

Engineering the electronic properties of heterogeneous photocatalysts with charge transfer regulated is an effective strategy to boost their CO2 reduction activity. Here, we drew inspiration from the strong metal-support interaction effect, and fabricated ZnIn2S4 supported-Cu sub-nanometric clusters photocatalyst. Within this catalyst, the formed CuS bond would redistribute interfacial charge, resulting in diverse chemical states of Cu atoms and the establishment of Ohmic contact between ZIS and Cu. The built-in electric field of such Ohmic contact benefited the migration of photoexcited electrons from ZIS to Cu. Further mechanistic studies unveiled the crucial role of positively charged Cu atom near the interface in facilitating H2O dissociation, and its adjacent Cu atom at the top-surface adopting a distinct chemical state could activate linear CO2 molecule into a bent configuration. These features substantially lowered energy barriers for CO2 adsorption and subsequent *COOH formation, and Cu-ZIS, accordingly, exhibited a remarkable CO production rate of 60.2 μmol g-1h−1, approximately 20.8-fold enhancement compared to ZIS counterpart.

Two-Orders-of-Magnitude Enhancement of SERS Activity via a Simple Surface Engineering of Quasi-Metal Single-Crystal Frameworks.

Beyond noble metals and semiconductors, quasi-metals have recently been shown to be noteworthy substrates for surface enhanced Raman spectroscopy, and their excellent quasi-metal surface-enhanced Raman spectroscopy (SERS) sensing has demonstrated a wider range of application scenarios. However, the underlying mechanism behind the enhanced Raman activity is still unclear. Here, we demonstrate that surface hydroxyls play a crucial role in the enhancement of the SERS activity of quasi-metal nanostructures. As a demonstration material, quasi-metallic MoO2 single-crystal frameworks rich in surface hydroxyls have been shown to have 100 times higher SERS activity than MoO2 single-crystal frameworks without hydroxyl functionalization, with a Raman enhancement factor of up to 7.6 × 107. Experimental and first-principles density-functional theory calculation results show that the enhanced Raman activity can be attributed to an effective interfacial charge transfer within the MoO2/OH/molecule system.

Interface coupling to improve O2 adsorption and accelerate charge separation for boosting photocatalytic performance of ZnO/ZnIn2S4 composite in H2O2 production and environmental remediation

The key to heterogeneous photo-Fenton technology lies in the efficient generation of hydrogen peroxide (H2O2). Herein, a newly-designed ZnO/ZnIn2S4 composite with heterostructure is synthesized. Benefiting from the formation of built-in electric field, the recombination of photoinduced electrons and holes is suppressed and interfacial charge transfer resistance is reduced. Importantly, the embedding of ZnO in ZnIn2S4 can improve the hydrophobicity and create microscopic three-phase interface, thereby boosting the capture capability for O2 and providing the convenience for the occurrence of O2 reduction reaction. More interestingly, the existence of ZnIn2S4 in the ZnO/ZnIn2S4 composite can reduce the Gibbs free energy (ΔG) of key intermediate (OOH*) formation, which will accelerate the generation of H2O2. As a result, the ZnO/ZnIn2S4 composite displays excellent performance in photocatalytic H2O2 production, and the highest yield was about 897.6 μmol/g/h within 60 min under visible light irradiation. The transfer of photoinduced carriers follows the S-scheme type mechanism. The photogenerated holes can be captured by drug residues (i.e., diclofenac sodium) to accelerate H2O2 production, while generated H2O2 can combine with Fe2+ to construct photo-Fenton system for achieving the advanced degradation of diclofenac sodium, which was mainly related to the formation of OH•. Furthermore, generated H2O2 can be applied for performing the inactivation of pathogenic bacteria. In short, current work will provide a valuable reference for future research.

Hydrogen Bonds and In situ Photoinduced Metallic Bi0/Ni0 Accelerating Z‐Scheme Charge Transfer of BiOBr@NiFe‐LDH for Highly Efficient Photocatalysis

AbstractFor heterojunction system, the lack of stable interfacial driving force and definite charge transfer channel makes the charge separation and transfer efficiency unsatisfactory. The photoreaction mechanism occurring at the interface also receives less attention. Herein, a 2D/2D Z‐scheme junction BiOBr@NiFe‐LDH with large‐area contact featured by short interface hydrogen bonds and strong interfacial electric field (IEF) is synthesized, and in situ photoinduced metallic species assisting charge transfer mechanism is demonstrated. The hydrogen bonds between O atoms from BiOBr and H atoms from NiFe‐LDH induce a significant interfacial charge redistribution, establishing a robust IEF. Notably, during photocatalytic reaction, Bi0 and Ni0 are in situ performed in heterojunction, which separately act as electron transport mediator and electron trap to further accelerate charge transfer efficiency up to 71.2 %. Theoretical calculations further demonstrate that the existence of Bi0 strengthens the IEF. Therefore, high‐speed spatial charge separation is realized in Bi0/BiOBr@Ni0/NiFe‐LDH, leading to a prominent photocatalytic activity with a tetracycline removal ratio of 88.3 % within 7 min under visible‐light irradiation and the presence of persulfate, far exceeding majority of photocatalysts reported previously. This study provides valid insights for designing hydrogen bonding heterojunction systems, and advances mechanistic understanding on in situ photoreaction at interfaces.

Promoting Reaction Kinetics and Boosting Sodium Storage Capability via Constructing Stable Heterostructures for Sodium‐Ion Batteries

AbstractConstructing heterostructures containing multiple active components is proven to be an efficient strategy for enhancing the sodium storage capability of anode materials in sodium‐ion batteries (SIBs). However, performance enhancement is often attributed to the unclear synergistic effects among the active components. A comprehensive understanding of the reaction mechanisms on the interfaces at the atomic level remains elusive. Herein, the carbon‐coated Fe3Se4/CoSe (Fe3Se4/CoSe‐C) anode material as a model featuring atomic‐scale contact interfaces is synthesized. This unique heterogeneous architecture offers an adjustable electronic structure, which facilitates rapid reaction kinetics and enhances structural integrity. In situ microscopic and ex situ spectral characterization techniques, along with theoretical simulations, confirm that the heterointerface with strong electric fields promotes Na+ ion migration. Based on solid‐state nuclear magnetic resonance (NMR) analysis, an interface charge storage mechanism is revealed, resulting in the enhanced specific capacity of the anode materials. When employed as an anode in SIBs, the Fe3Se4/CoSe‐C electrode demonstrates excellent rate capabilities (218 mAh g−1 at 7 A g−1) and prolonged cycling stability (258 mAh g−1 at 5 A g−1 after 1000 cycles). This work highlights the significance of heterointerface engineering in electrode material design for rechargeable batteries.