Intimate Interface Research Articles

Silver Nanoparticles In Situ Enhanced Electrochemiluminescence of the Porphyrin Organic Matrix for Highly Sensitive and Rapid Monitoring of Tetracycline Residues.

Accurate monitoring of tetracycline (TC) residues in the environment is crucial for avoiding contaminant risk. Herein, a novel TC biosensor was facilely designed by integrating silver nanoparticles (Ag NPs) into the porphyrin metal-organic matrix (Ag@AgPOM) as a bifunctional electrochemiluminescence (ECL) probe. Different from the step-by-step synthesis of the co-reaction accelerator and ECL emitter, the co-reaction accelerators Ag NPs were in situ-grown on the surface of 5,10,15,20-tetrakis (4-carboxyphenyl) porphyrin (TCPP) via a simple one-pot approach. Symbiotic Ag NPs on Ag@AgPOM formed an intimate interface and increased the collision efficiency of the ECL reaction, achieving the ECL enhancement of TCPP. Under the optimized conditions, the ternary ECL biosensor showed a wide linear detection range toward TC with a low detection limit of 0.14 fmol L-1. Compared with the traditional HPLC and ELISA methods, satisfied analytical adaptability made this sensing strategy feasible to monitor TC in complex environmental samples.

Mechanism insight into boosting photocatalytic purification of tetracycline hydrochloride over 2D/2D S-scheme (BiO)2CO3/BiOCl heterojunctions

The (BiO)2CO3/BiOCl heterojunction holds promise for photocatalytic purification of antibiotics, which is primarily attributed to the type-II and Z-scheme photocharge separation mechanisms. However, it lacks a report on S-scheme heterojunction for efficiently promoting photocharge separation and retaining powerful redox capability. In this study, a 2D/2D S-scheme (BiO)2CO3/BiOCl (denoted as (BC/BL)1) heterojunction was prepared through the hydrothermal synthesis method. The as-synthesized (BC/BL)1 exhibited a significantly enhanced photocatalytic activity, with a degradation rate of tetracycline hydrochloride (TC-HCl) reaching 95.3% after 60 minutes. Its kinetic constant of photodegradation surpassed that of (BiO)2CO3 and BiOCl by 20.8 and 3.8 times, respectively. A series of characterizations revealed that the improved photocatalytic activity of the (BC/BL)1 sample stemmed from the formation of a built-in electric field at the intimate interface, which strongly drove the photogenerated carriers to achieve the S-scheme separation. This study highlights the potential application prospects of photocatalyst (BC/BL)1 in antibiotic degradation.

Unlocking photocatalytic NO removal potential in an S‐type UiO‐66‐NH2/ZnS(en)0.5 heterostructure

AbstractThe contamination of nitric oxide presents a significant environmental challenge, necessitating the development of efficient photocatalysts for remediation. Conventional heterojunctions encounter obstacles such as large contact barriers, sluggish charge transport, and compromised redox capacity. Here, we introduce an innovative S‐type heterostructure photocatalyst, UiO‐66‐NH2/ZnS(en)0.5, designed specifically to overcome these challenges. The synthesis, employing a unique microwave solvothermal method, strategically aligns the lowest unoccupied molecular orbital of UiO‐66‐NH2 with the highest occupied molecular orbital of ZnS(en)0.5, fostering the formation of a stepped heterojunction. The resulting intimate interface contact generates a built‐in electric field, facilitating charge separation and migration, as evidenced by time‐resolved photoluminescence spectroscopy and photoelectrochemical tests. The abundant active sites in the porous UiO‐66‐NH2 counterpart provide adsorption and activation sites for nitrogen monoxide (NO) oxidation. Performance evaluation reveals exceptional photocatalytic NO removal, achieving 70% efficiency and 99% selectivity toward nitrates under simulated solar illumination. Evidence from X‐ray photoelectron spectroscopy and trapping experiments supports the effectiveness of the S‐type heterostructure, showcasing refined reactive oxygen species, particularly superoxide. Thus, this study introduces a new perspective on advanced NO oxidation and unlocks the potential of S‐scheme heterojunctions to refine reactive oxygen species for NO remediation.

In situ anchoring of Ni12P5 on ZnIn2S4 for efficient and stable photocatalytic H2 evolution

It is a great challenge to develop efficient, stable and inexpensive hydrogen evolution reaction (HER) catalysts for photocatalytic water-splitting. In this paper, Ni12P5 (NP) was in situ anchored on the surface of ZnIn2S4 (ZIS) via a solvothermal route with nickel chloride and red phosphorus as ingredients. Using triethanolamine as sacrificial agent, the photocatalytic hydrogen evolution activity of NP/ZIS was studied under visible light irradiation. At the same time, the composition, structure, morphology and photoelectrochemical properties of the as-obtained samples were analyzed through a sequence of characterization techniques. ZIS loaded with 6 wt% NP (6NP/ZIS) exhibits the best hydrogen evolution activity and excellent stability. The H2 evolution rate of 6NP/ZIS is 5.4 times higher than that of pristine ZIS and well beyond that of the physical mixture (6NP + ZIS) or even that of the optimal Pt/ZIS under the same conditions. The maximal apparent quantum yield (AQY) of 22.7 % at 400 nm is achieved, superior to the most reported performance of ZnIn2S4-based photocatalysts for HER. The anchor of NP can not only enhance the visible light absorption intensity, but also reduce the HER overpotential. More importantly, the intimate interface between ZIS and NP can promote the separation and migration of photo-excited carriers, thereby enhancing the activity of photocatalytic hydrogen evolution. The possible photocatalytic reaction mechanism was discussed.

Hierarchical LaTiO2N/Sn3O4 heterojunction with intimate interface contact for enhanced photocatalytic water splitting

LaTiO2N/Sn3O4 heterojunction with type-II band structure and hierarchical microstructure was constructed by decorating Sn3O4 nanoflowers and nanoflakes intimately on the surface of LaTiO2N nanosheets via a facile hydrothermal method. Compared with pure Sn3O4 and bare LaTiO2N, the photocatalytic H2 evolution activity for LaTiO2N/Sn3O4 heterostructure was boosted by ∼3 and ∼52 times, respectively, reaching 887 μmol·h−1·gcat−1. The mechanism for the elevated photocatalytic performance was systematically disclosed on the basis of comprehensive characterizations. Specifically, the introduced LaTiO2N extended the visible light absorption range to ∼600 nm, endowing Sn3O4 with more photogenerated charge carriers. Subsequently, the type-II band structure expedited the separation and migration of charge carriers, diminishing the internal recombination, thereby enhancing the photocatalytic activity. This work affords a new avenue for designing tin oxide-based and oxynitrides-based heterojunction.

In Situ Construction of Interface with Photothermal and Mutual Catalytic Effect for Efficient Solar-Driven Reversible Hydrogen Storage of MgH2.

Hydrogen storage in MgH2 is an ideal solution for realizing the safe storage of hydrogen. High operating temperature, however, is required for hydrogen storage of MgH2 induced by high thermodynamic stability and kinetic barrier. Herein, flower-like microspheres uniformly constructed by N-doped TiO2 nanosheets coated with TiN nanoparticles are fabricated to integrate the light absorber and thermo-chemical catalysts at a nanometer scale for driving hydrogen storage of MgH2 using solar energy. N-doped TiO2 is in situ transformed into TiNxOy and Ti/TiH2 uniformly distributed inside of TiN matrix during cycling, in which TiN and Ti/TiHx pairs serve as light absorbers that exhibit strong localized surface plasmon resonance effect with full-spectrum light absorbance capability. On the other hand, it is theoretically and experimentally demonstrated that the intimate interface between TiH2 and MgH2 can not only thermodynamically and kinetically promote H2 desorption from MgH2 but also simultaneously weaken Ti─H bonds and hence in turn improve H2 desorption from the combination of weakened Ti─H and Ti─H bonds. The uniform integration of photothermal and catalytic effect leads to the direct action of localized heat generated from TiN on initiating the catalytic effect in realizing hydrogen storage of MgH2 with a capacity of 6.1wt.% under 27 sun.

Artificially regulating the crystallinity for constructing poly(heptazine imide)-based S-scheme homojunction with boosted photocatalytic hydrogen evolution performance

Fabricating homojunction photocatalyst is a promising approach to accelerate the separation and transfer of photogenerated charge carriers, and to boost photocatalytic performance. Herein, a novel poly (heptazine imide) (PHI)-based S-scheme homojunction photocatalyst (U/T-LHPHI) is fabricated through an ionothermal synthesis route, which exhibits particular high and low crystallinity property, intimate interface combination, and locally N self-doping. The regulation of crystallinity contributes to the differentiated electronic structure in PHI, which leads to the establishment of internal electric field (IEF). The intense IEF and N doping level with electron extracting capacity synergistically promote the charge transfer from the high crystalline PHI (HPHI) to the low crystalline PHI (LPHI) following the S-scheme mechanism. Additionally, the strong interfacial interaction improves the interfacial charge transfer dynamics. As a consequence, photogenerated electrons with powerful reducing ability are maintained effectively. Upon light irradiation, the optimized U/T-LHPHI performs an H2 evolution rate of 4880, 2416, and 2375 µmol g−1 h−1 in deionized water, simulated seawater, and real seawater, respectively, which exceed that of many carefully designed noble metal Pt containing photocatalyst. This work provides an important verification that the rational design and construction of homojunction photocatalysts could effectively enhance photocatalytic activity.

Double‐Helical Carbon Nanotube‐Wrapped Elastomeric Mandrel for Electrical Shortage‐Free, One‐Body Multifunctional Fiber Systems

AbstractSoft and elastic fiber‐based electronic devices exhibiting high electromechanical stability are highly desirable for sustainable and continuous utilization in various applications. However, effectively assembling the cathode and anode in a single body without unwanted interconnections and realizing an intimate contact interface between the electrode and substrate remain challenging. Here, an electrical shortage‐free one‐body fiber system with double‐helix buckle electrodes created by torsion‐ and strain‐mismatch between carbon nanotube (CNT) ribbons and a rubber substrate is reported. The as‐used CNT ribbons serve as the strain‐insensitive electrode, while the rubber mandrel‐core fiber acts as the key matrix in the following three aspects: as an elastic substrate that ensures reversible structural changes during mechanical deformations; as a dielectric layer for capacitive strain sensing; and as an electrothermal expansion element for tensile contraction. Moreover, because of the mismatch‐induced torque‐balance structure, the helically wrapped CNT buckle electrodes can effectively absorb the applied stresses without noticeable delamination and electrical conductance loss. Consequently, the double‐helix buckle fiber system can reliably provide multiple functions, viz. detection of various deformations (e.g., stretching, twisting, and pressing), electrochemical energy storage with excellent strain tolerance, and reversible electrothermal tensile actuation.

Ultrathin Reed Membranes: Nature's Intimate Ion‐Regulation Skins Safeguarding Zinc Metal Anodes in Aqueous Batteries

AbstractThe practical realization of aqueous zinc‐ion batteries relies crucially on effective interphases governing Zn electrodeposition chemistry. In this study, an innovative solution by introducing an ultrathin (≈2 µm) biomass membrane as an intimate artificial interface, functioning as nature's ion‐regulation skin to protect zinc metal anodes is proposed. Capitalizing on the inherent properties of natural reed membrane, including multiscale ion transport tunnels, abundant ─OH groups, and remarkable mechanical integrity, the reed membrane demonstrates efficacy in regulating uniform and rapid Zn2+ transport, promoting desolvation, and governing Zn (002) plane electrodeposition. Importantly, a unique in situ electrochemical Zn─O bond formation mechanism between the reed membrane and Zn electrode upon cycling is elucidated, resulting in a robustly adhered interface covering on the zinc anode surface, ultimately ensuring remarkable dendrite‐free and highly reversible Zn anodes. Consequently, the approach achieves a prolonged cycle life for over 1450 h at 3 mA cm−2/1.5 mAh cm−2 in symmetric Zn//Zn cells. Moreover, exceptional cyclic performance (88.95%, 4000 cycles) is obtained in active carbon‐based cells with an active mass loading of 5.8 mg cm−2. The approach offers a cost‐effective and environmentally friendly strategy for achieving stable and reversible zinc anodes for aqueous batteries.

Hybrid hard carbon framework derived from polystyrene bearing distinct molecular crosslinking for enhanced sodium storage

AbstractExploiting high‐performance yet low‐cost hard carbon anodes is crucial to advancing the state‐of‐the‐art sodium‐ion batteries. However, the achievement of superior initial Coulombic efficiency (ICE) and high Na‐storage capacity via low‐temperature carbonization remains challenging due to the presence of tremendous defects with few closed pores. Here, a facile hybrid carbon framework design is proposed from the polystyrene precursor bearing distinct molecular bridges at a low pyrolysis temperature of 800°C via in situ fusion and embedding strategy. This is realized by integrating triazine‐ and carbonyl‐crosslinked polystyrene nanospheres during carbonization. The triazine crosslinking allows in situ fusion of spheres into layered carbon with low defects and abundant closed pores, which serves as a matrix for embedding the well‐retained carbon spheres with nanopores/defects derived from carbonyl crosslinking. Therefore, the hybrid hard carbon with intimate interface showcases synergistic Na ions storage behavior, showing an ICE of 70.2%, a high capacity of 279.3 mAh g−1, and long‐term 500 cycles, superior to carbons from the respective precursor and other reported carbons fabricated under the low carbonization temperature. The present protocol opens new avenues toward low‐cost hard carbon anode materials for high‐performance sodium‐ion batteries.

Facilitating charge separation by constructing CuInS2/PCN S-scheme heterojunction with the intimate contact interface for enhanced photocatalytic CO2 reduction

Photocatalytic CO2 conversion efficiency is still much lower than what is expected owing to the sluggish charge separation and transfer for many semiconductors. Herein, we fabricated a highly efficient S-scheme heterojunction by integrating the CuInS2 (CIS) with the oxygen-doping brown polymer carbon nitride (PCN). The construction of CIS/PCN S-scheme heterojunction promotes spatial separation of photogenerated charge while maintaining their strong reduction capability. The formed intimate contact interface between the CIS and PCN provides the strong driving force for the transfer of photogenerated charge, which accelerates the electrons rapidly migrating from PCN to CIS through the tight interface, resulting in more reductive electrons participating in photocatalytic reaction. As a result, the CIS/PCN S-scheme heterostructure shows a remarkably enhanced photocatalytic activity with a CO yield rate of up to 105.89 μmol g-1h−1, which is 7 times higher than that of the CIS. Combined density functional theory (DFT) calculations with experimental results demonstrate the formation of an intimate contact interface is not only more conducive to CO2 adsorption and activation but also lowers the reaction energy barrier of the conversion of CO2 to CO. Meanwhile, ESR characterization reveals the electron transfer pathway of CIS/PCN for photocatalytic CO2 conversion. This work may provide an illuminating insight into designing the S-scheme photocatalyst for enhanced CO2 photoreduction.

Multi-synergies of hollow CdS cubes on MoS2 sheets for enhanced visible-light-driven photocatalysis

Formation of intimate interfaces in semiconductor-based heteronanostructures (HNSs) is widely adopted to enhance the efficiency of photocatalytic hydrogen evolution via water splitting because of their efficient light harvesting, charge carrier separation, and transfer capability originating from intimate interface. Here, we employ a multi-step approach, involving the direct growth of the photocatalytically active semiconductor (Cu2O) on MoS2 sheets, along with anion exchange and cation exchange methods to design hollow CdS cube/MoS2 sheet HNSs (H-CdS/MoS2 HNSs) consisting of intimate interfaces between hollow CdS cubes and MoS2 sheets. These distinctive morphological and compositional features endow H-CdS/MoS2 HNSs with exceptional charge transfer capability, intrinsic catalytic activity, and light-harvesting capacity. Consequently, H-CdS/MoS2 HNSs demonstrate significantly enhanced photocatalytic performance and stability for hydrogen evolution reactions and pollutant degradation under visible light irradiation compared to their binary and unary photocatalyst counterparts. This design strategy demonstrates the significance of forming intimate interfaces using hollow semiconductors in HNSs for advanced photocatalysis.

Grinding preparation of 2D/2D g-C3N4/BiOCl with oxygen vacancy heterostructure for improved visible-light-driven photocatalysis

A novel 2D/2D g-C3N4/BiOCl (CN/BOC) heterojunction photocatalyst was synthesized by grinding appropriate amounts of CN, Bi(NO3)3·5H2O, glacial acetic acid and KCl at room temperature. The porous CN nanosheets not only facilitate the in situ nucleation and growth of BOC to form thin nanosheets and constitute an intimate contact interface, but also introduce more oxygen vacancies (OVs) in the grinding process. The 2D/2D CN/BOC heterojunction had a good interface and generates a built-in electric field, which can improve the separation of e− and h+. The synergistic effect of the heterostructure and OVs made the photocatalyst have significantly better performance than CN and BOC alone under visible light. The most efficient CN/BOC-5 could achieve a tetracycline (TC) degradation rate of 89.8% within 2 h, which was 1.9 and 1.2 times faster than CN and BOC, respectively. It catalyzed the reduction of CO2 to CO at a rate of 2.00 μ mol h−1 g−1, 1.1 and 3.2 times faster than CN and BOC, respectively. The mechanism for the photocatalysis of CN/BOC-5 was revealed. It was confirmed that the efficiency of photo-induced carrier separation and visible-light photo-absorption were both considerably increased by the synergistic interaction between OVs and 2D/2D heterojunction. This research may open up new possibilities for the logical design of efficient photocatalysts through combining 2D/2D heterojunctions with OVs for environmental remediation.Graphical

Hydrochar-Supported NiFe2O4Nanosheets with a Tailored Microstructure for Enhanced CO2Photoreduction to Syngas.

Constructing high-efficiency composite photocatalysts with enhanced charge transfer and a rapid surface catalytic reaction has recently received significant attention. Herein, a hydrochar-mediated NiFe2O4 nanosheet (C/NFO) composite was rationally constructed by a simple hydrothermal method. Intimate interface contacts and chemical interactions between hydrochar and NFO were formed. The prepared C/NFO samples exhibited remarkable visible-light-driven catalytic CO2 reduction properties under mild reaction conditions with Ru(bpy)32+ sensitization. As the optimized sample, 16%-C/NFO achieved a 4-fold enhancement of CO production (17.49 μmol/h) compared with that of pure NFO. The C/NFO samples demonstrated good activity and structural stability in the CO2 photoreduction system. The carbon source of CO derived from CO2 was verified through isotopic labeling experiments using 13CO2. In situ photoluminescence and electrochemical characterizations confirmed the role of electron transfer intermediates of C/NFO. The synergistic effect of the nanosheet-like structure of NFO, combined with the surface functional groups of hydrochar, facilitated an exceptionally high rate of charge transfer and exposed abundant active adsorption sites for CO2, thereby promoting the efficient separation of photogenerated charge carriers and enhancing photocatalytic activity for CO2 reduction. This study presents a promising strategy for the rational design of hydrochar coupled with transition metal compound catalysts for efficient CO2 photoreduction.

Construction of an interpenetrating manganese residue-derived FeC2O4/CuC2O4 composite with enhanced charge transfer in photo-Fenton reactions via mechanical activation pre-anchoring strategy

The low rates of charge separation and migration and the pronounced photo-corrosion of FeC2O4 significantly limit its environmental applications. Strengthening the charge transfer rate by constructing a tight bimetallic interface is an attractive method. Herein, a novel interpenetrating manganese residue (MR)-derived FeC2O4/CuC2O4 (MAMR-FeCuOx) composite with intimate interface was constructed via mechanical activation (MA) pre-anchoring and liquid-phase deposition-photo-reduction strategy, and was used as a photo-Fenton catalyst for efficient degradation of oxytetracycline (OTC) under visible light irradiation. The Cu2+ was uniformly dispersed and anchored on the surface of MR after MA pretreatment and an interpenetrating structure was formed through the liquid-phase deposition-photo-reduction process. MAMR-FeCuOx displayed excellent photo-Fenton catalytic performance and stability with a 99% OTC removal rate within 10 min, which is 20.87 times higher than that of FeC2O4, and maintained over 96% OTC removal rate even after ten consecutive cycles. These enhanced catalytic performances and stability can be attributed to the formation of an interpenetrating structure with the intimate interface between FeC2O4 and CuC2O4 induced by MA pretreatment, which promoted electronic interactions between Fe and Cu for effectively reducing the charge transfer barriers. This improved the utilization rate of visible light, the interface electron migration, and the separation efficiency of photogenerated charge carriers. This study provides new insights into the valorization of solid waste and the development of stable and efficient FeC2O4-based catalysts.

Zinc-doped C4N3/BiOBr S-scheme heterostructured hollow spheres for efficient photocatalytic degradation of tetracycline.

Photocatalytic degradation of organic pollutants in water is of great significance to the sustainable development of the environment, but encounters limited efficiency when a single compound is used. Thus, there have been enormous efforts to find novel photocatalytic heterostructured composites with high performance. In this work, a novel S-scheme heterostructure is constructed with BiOBr and Zn2+ doped C4N3 (Zn-C4N3) by a solvothermal method for efficient photodegradation of tetracycline (TC), a residual antibiotic difficult to be removed from the aquatic environment. Thanks to Zn2+-doping induced improvement in chemical affinity between Zn-C4N3 and BiOBr, well-formed Zn-C4N3/BiOBr heterostructured hollow spheres are formed. This structure can efficiently suppress fast recombination of photogenerated electron-hole pairs to enhance the photocatalytic activity of BiOBr dramatically. At a room temperature of 25 °C and neutral pH 7, the catalyst can degrade a significant portion of TC pollutants within 30 min under visible light. Also, the Zn-C4N3/BiOBr heterostructure displays good stability after recycling experiments. Free radical capture experiments and ESR tests show that ˙O2- is the main active substance for photocatalytic degradation of TC. This study provides new insights for constructing heterostructures with an intimate interface between the two phases for photocatalytic applications.

From one to two: in situ construction of C3N5-poly(triazine imide) heterojunction for enhanced O2 activation.

A novel C3N5-poly(triazine imide) (PTI) heterojunction was designed and constructed using a thermal polymerization process, and featured an intimate S-scheme interface coupling and a particularly good performance for H2O2 production. This work provides a new perspective for constructing metal-free C3N5-based heterojunctions to be used for selective molecular oxygen activation.

(Invited) Towards Broadband Photocatalysis

Forming nanomaterials junctions and using plasmons represent two important, promising strategies for realizing broadband photocalysis in strategically important applications such as solar fuels and photocatalytic degradation of pollutants. In this talk, I will present some of our recent work on the rational design of nanohybrids and their applications in solar fuels and photocatalysis. One example is about the in situ synthesis of plasmonic Ag nanoparticles (AgNPs) and Ag-MOF. The intimate and stable interface between the AgNPs and Ag-MOF and hot electron transfer from the plasmonic AgNPs to MOF led to highly efficient visible-light photocatalytic H2 generation in aqueous solution, which surpasses most of reported MOF-based photocatalytic systems. This work sheds light on effective electronic and energy bridging between plasmonic NPs and MOF.

Crystal Orientation-Dependent Interface Compatibility in the Oxide Composite Cathode by in Situ Heating Transmission Electron Microscopy

All-solid-state batteries (ASSBs) with oxide-based solid electrolytes are getting prominence as a forthcoming battery system capable of overcoming the drawbacks of current lithium-ion batteries by satisfying the expanding demand for high energy density and safety. However, the poor interfacial contact between cathode active materials and solid electrolytes, at which lithium ions diffuse and the charge transfer occurs, is a major concern for practical utilization. Although the co-sintering process at high temperatures is essential to achieve an intimate interface contact, excessive thermal energy reversely accelerates the interfacial degradation reaction, of which the mechanism has been still unexplored. Here, using an epitaxial model system in which the crystal orientations of the Li(Ni1/3Co1/3Mn1/3)O2 cathode and Li3xLa(2/3)-x⎕(1/3)-2xTiO3 solid electrolyte are controlled, we directly probe the interfacial reaction in real-time during heating by in situ heating transmission electron microscopy, and investigate the impact of the crystal orientation at the interface on the interfacial reaction mechanism and kinetics. In situ observation reveals that the interfacial reactions are highly dependent on the crystal orientation at the interface involving the onset temperature of the reaction, the diffusion behavior of lithium ions, the intermediate states, and the overall degradation mechanism between the active material and the solid electrolyte. The interfacial degradation during heating increases the charge transfer resistance between the cathode active material and the solid electrolyte, and the increasing tendency of the resistance is closely related to the crystal orientation-dependent interfacial degradation.

Construction of embedded CdS nanosheets@PEA2PbBr4 nanoplate p-n heterojunction photocatalysts with spatial charge transfer for enhanced benzylic C(sp3)-H bond oxidation

Metal halide perovskites (MHP) have emerged as promising new-generation photocatalysts due to their exceptional photoelectric properties. Here, we for the first time fabricate a novel CdS nanosheets@PEA2PbBr4 nanoplate p-n heterojunction using a simple anti-solvent method for photocatalytic activation of benzylic C(sp3)-H bond. The in-situ fabrication strategy enables the rapid growth of PEA2PbBr4 nanoplate to envelop the CdS nanosheets that serve as nucleation sites. This results in an embedded structure with large and intimate contact interface, providing abundant charge transfer channels. Additionally, the staggered band structure coupled with large difference in Fermi levels between the p-PEA2PbBr4 and the n-CdS form a strong internal electric field (IEF) that greatly accelerates the migration and realizes spatial separation of photoinduced electrons and holes within the heterojunction. Under visible light irradiation, the CdS@PEA2PbBr4 heterojunction displays notably improved photocatalytic C(sp3)-H bond oxidation activity. The optimized 5 % CdS@PEA2PbBr4 catalyst demonstrates a benzaldehyde (BAD) production rate of 4320 μmol g−1h−1, which is 5-folds higher than that of pure PEA2PbBr4 (950 μmol g−1h−1), and 18-folds greater than the blank CdS (240 μmol g−1h−1). Mechanistic study reveals that h+, O2− and 1O2 are the main active species contributing to C(sp3)-H bond oxidation. This work not only presents the first photocatalytic application of PEA2PbBr4, but also offers insights for developing MHP-based in-situ heterojunctions with desired nanostructure to further enhance photocatalytic performance.