Separation Of Photogenerated Carriers Research Articles

Insights on the efficiency and contribution of single active species in photocatalytic degradation of tetracycline: Priority attack active sites, intermediate products and their toxicity evaluation

Photocatalysis has been proven to be an excellent technology for treating antibiotic wastewater, but the impact of each active species involved in the process on antibiotic degradation is still unclear. Therefore, the S-scheme heterojunction photocatalyst Ti3C2/g-C3N4/TiO2 was successfully synthesized using melamine and Ti3C2 as precursors by a one-step calcination method using mechanical stirring and ultrasound assistance. Its formation mechanism was studied in detail through multiple characterizations and work function calculations. The heterojunction photocatalyst not only enabled it to retain active species with strong oxidation and reduction abilities, but also significantly promoted the separation and transfer of photo-generated carriers, exhibiting an excellent degradation efficiency of 94.19 % for tetracycline (TC) within 120 min. Importantly, the priority attack sites, degradation pathways, degradation intermediates and their ecological toxicity of TC under the action of each single active species (·O2−, h+, ·OH) were first positively explored and evaluated through design experiments, Fukui function theory calculations, HPLC-MS, Escherichia coli toxicity experiments, and ECOSAR program. The results indicated that the preferred attack sites of ·O2− on TC were O20, C7, C11, O21, and N25 atoms with high f+ value. The toxicity of intermediates produced by ·O2− was also lower than those produced by h+ and ·OH.

A hydrogen sulfide photoelectrochemical sensor based on BiVO4/Fe2O3 heterojunction.

A BiVO4/Fe2O3 heterojunction for non-enzymatic photoelectrochemical (PEC) determination of hydrogen sulfide (H2S) is reported. The BiVO4/Fe2O3 heterojunction promoted the separation of photo-generated carriers, reduced electron-hole recombination, and thus improved electron collection and photocurrent. The proposed BiVO4/Fe2O3/FTO sensor exhibited a linear range of 1-500μM and a detection limit of 0.51 nMH2S. In addition, high selectivity, good reproducibility, and stability were obtained for H2S sensing. Thedetection of H2S in water and serum samples demonstrated its feasibility. This work provides a new strategy to detect and understand the bio-function of H2S in the biological environment.

Constructing Metal-Organic Framework Films with Adjustable Electronic Properties on Hematite Photoanode for Boosting Photogenerated Carrier Transport.

Hematite (α-Fe2O3) has become a research hotspot in the field of photoelectrochemical water splitting (PEC-WS), but the low photogenerated carrier separation efficiency limits further application. The electronic structure regulation, such as element doping and organic functional groups with different electrical properties, is applied to alleviate the problems of poor electrical conductivity, interface defects, and band mismatch. Herein, α-Fe2O3 photoanodes are modified to regulate their electric structures and improve photogenerated carrier transport by the bimetallic metal-organic frameworks (MOFs), which are constructed with Fe/Ni and terephthalate (BDC) with 2-substitution of different organic functional groups (─H, ─Br, ─NO2 and ─NH2). The α-Fe2O3 photoanode loaded with FeNi-NH2BDC MOF catalyst exhibits the optimal photocurrent density (2mAcm-2) at 1.23VRHE, which is 2.33 times that of the pure α-Fe2O3 photoanode. The detailed PEC analyses demonstrate that the bimetallic synergistic effect between Fe and Ni can improve the conductivity and inhibit the photogenerated carrier recombination of α-Fe2O3 photoanodes. The ─NH2 group as an electron-donor group can effectively regulate the electron distribution and band structure of α-Fe2O3 photoanodes to prolong the lifetime of photogenerated holes, which facilitates photogenerated carrier transport and further enhances the PEC-WS performance of α-Fe2O3 photoanode.

Strongly active and environmentally friendly WO3/C3N4 photocatalysts for converting cyclohexane to cyclohexanone under ambient conditions

C–H bond activation under mild conditions remains a great challenge in the chemical industry, while catalytic cyclohexane oxidation is inefficient and often requires organic solvents and strong oxidants. This study constructed a C3N4/WO3 Z-type heterojunction catalyst to efficiently convert cyclohexane into cyclohexanone and cyclohexanol (KA oil) through aqueous phase oxidation by O2 under visible light irradiation. With strong redox performance and high photogenerated carrier separation ability, the proposed composite catalyst can produce the key active species for cyclohexane oxidation in the H2O–O2 system. The reaction mechanism was clarified through experiment and DFT theory calculation. Cyclohexane was converted into cyclohexyl radical under the action of ·OH, and ·O2− converted most products into cyclohexanone. The catalyst can be recycled under optimized process conditions while reaching a KA oil yield of 139.73 μmol g−1 h−1 and a selectivity of 93.1%.

Magnetic-supported catalyst derived from red mud-based Fe-Co PBA for efficient degradation of organic pollutants by activating peroxymonosulfate under visible light

To alleviate the environmental pressure caused by the continuous accumulation of solid waste red mud (RM) and organic pollutants, we developed a magnetic-supported catalyst derived from RM-based Fe-Co Prussian blue analogues (RM-Co PBA-D) using RM as the iron source and carrier. Then, the catalyst was used to activate peroxymonosulfate (PMS) under visible light for the degradation of tetracycline (TC) and rhodamine B (RhB). Due to the superior dispersion, strong visible light response, and high photo-generated carrier separation efficiency of the RM-Co PBA-D, the RM-Co PBA-D/PMS/Vis system could completely degrade both TC (10 mg/L) and RhB (20 mg/L) in 30 min, with mineralization efficiencies as high as 70.12 % and 60.59 %, respectively. Several reactive oxygen species (ROS) such as SO4⋅−, ⋅OH−, ⋅O2−, 1O2, and h+ were involved in the degradation process, with SO4⋅− and 1O2 playing a dominant role. More importantly, except for the production of ROS, the regeneration of active sites (Co2+/Fe2+) mediated by photo-generated carriers was also a critical factor in enhancing the removal of organic pollutants. In addition, the constructed system demonstrated significant potential for practical applications, which was attributed to the stable structure and catalytic performance of the catalyst as well as the strong ability of the system to resist interference by impurity anions and detoxify organic pollutants.

Structure-controlled Interpenetrated MOF@COF via C-C Linkage for Enhanced Photocatalysis.

Diversifying the connecting junctions will be feasible for the controllable collaboration of metal organic frameworks (MOFs) and covalent organic frameworks (COFs) to rationally design multifunction-integrated heterostructures with enhanced performance, yet it is in the nascent stage. Herein, by intelligently exploiting the polymerization of vinyl group, C-C bond is innovatively introduced to construct the core-shell MOF@COF heterostructures with adjustable shell thickness and rare interpenetrated structure. The unique structure endows prepared C-C-linked MIL-68@COF-Vs with more superior visible-light harvesting and photogenerated carrier separation capability, leading to significantly higher photocatalytic activity and faster degradation rate than pristine MIL-68-C=Cs, COF-V, and imine-linked MIL-68-NH2@COF-V. Further, the customized MIL-68@COF-V is in-situ grown as reusable films with significantly boosted performance under ambient condition, which realize the highly efficient degradation of tetracycline within 15 min (96.5%), rhodamine 6G within 25 min (97.6%), and phenol within 40 min (95.3%) by solar drive. This work exhibits the distinctive advantages of C-C junction in the MOF@COF construction, and highlights the application prospect of rational-designed heterostructure in the treatment of persistent organic pollutants.

Precisely Regulating Asymmetric Charge Distribution by Single-Atom Central Doped Ag-Based Series Clusters for Enhanced Photoreduction of CO2 to Alcohol Fuels.

High efficiently photocatalytic CO2 reduction (CO2RR) into liquid fuels in pure water system remains challenged. Iron polyphthalocyanine (FePPc) with strong light harvesting, unique Fe-N4 structure, abundant pores, and good stability could serve as a promising catalyst for CO2 photoreduction. To further improve the catalytic efficiency, herein, symmetry-breaking Fe sites are constructed by coupling with atomically precise M1Ag24 (M=Ag, Au, Pt) series clusters. Especially, the introduction of Pt1Ag24 causes the most asymmetric charge distribution of Fe in FePPc (followed by Au1Ag24 and Ag25), leading to the favorable CO2 adsorption and activation. In addition, Pt1Ag24-FePPc exhibits the most effective photogenerated carriers transfer and separation. As a result, Pt1Ag24-FePPc shows the methanol/ethanol yield of 48.55/32.97 μmol·gcat-1·h-1 in H2O-CO2 system under visible light irradiation, ~ 1.65/1.25-fold, 1.83/1.37-fold, and 3.6/1.61-fold higher than that of Au1Ag24-FePPc, Ag25-FePPc, and FePPc, respectively. This work provides a concept for precisely construction and regulation symmetry-breaking sites of cluster-based catalysts for effective CO2 conversion.

W single-atom mediated singlet oxygen formation on carbon nitride for powerful photocatalytic abatement of organic pollutants

Active single-atom W anchoring on graphitic carbon nitride (g-C3N4) with interplanar four-coordination with N was achieved via a microwave hydrothermal process followed by thermal polymerization. The optimal monoatomic W incorporated g-C3N4 (W-CN) catalyst exhibited a high photocatalytic activity toward a wide range of pharmaceutical and personal care products (PPCPs). The anchoring of W single atom narrowed the energy-band, negatively shifted the conduction band of g-C3N4, and promoted the charge transfer and photogenerated carrier separation. Moreover, W single-atom intercalation obviously favored the formation of singlet oxygen (1O2), as validated by the active species capture test and density functional theory (DFT) calculation, which played an important role in the photocatalytic degradation of PPCPs. The treatment of actual wastewater, toxicity assessment and hemp-pea-growth experiments further showed that the W-CN photocatalyst could effectively degrade the organic pollutants and reduce their poisonousness in the water environment. This work offers a facile route to obtain reactive g-C3N4 with single-metal active sites and some insights into its activity enhancement for the abatement of organic pollutant-containing wastewater.

Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots‐g‐C3N4 Nanocomposites

AbstractThe extensive industrial applications of fuel oil, a critical strategic resource, are accompanied by significant environmental and health concerns due to the presence of sulfur‐containing compounds in its composition, which result in hazardous combustion waste. Extensive research has been conducted to develop technologies for low‐vulcanization fuel production to address this issue. Consequently, the investigation of catalysts for environmentally friendly and safe photocatalytic desulfurization becomes imperative. To that end, we have designed efficient MIL‐101(Fe)/CQDs@g‐C3N4 (MIL101/CDs‐C3N4) Z‐scheme heterojunction photocatalysts with high carrier separation and mobility through a thermal polymerization‐hydrothermal strategy. The high concentration of photogenerated carriers facilitates the activation of oxygen and H2O2, leading to increased production of ROS (⋅O2−, ⋅OH, h+), thereby enhancing the photocatalytic desulfurization (PODS). Additionally, DFT (Density functional theory) calculations were utilized to determine the electron migration pathways of the catalysts and adsorption energies of DBT (dibenzothiophene). Moreover, Gibbs free energy calculations indicated that MIL101/CDs‐C3N4 exhibited the lowest activation energy for oxygen and H2O2. The mechanism of photocatalytic desulfurization was proposed through a combination of theoretical calculations and experimental studies. This study provides guidance for the development of MOF‐based Z‐scheme systems and their practical application in desulfurization processes.

Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots-g-C3N4 Nanocomposites.

The extensive industrial applications of fuel oil, a critical strategic resource, are accompanied by significant environmental and health concerns due to the presence of sulfur-containing compounds in its composition, which result in hazardous combustion waste. Extensive research has been conducted to develop technologies for low-vulcanization fuel production to address this issue. Consequently, the investigation of catalysts for environmentally friendly and safe photocatalytic desulfurization becomes imperative. To that end, we have designed efficient MIL-101(Fe)/CQDs@g-C3N4 (MIL101/CDs-C3N4) Z-scheme heterojunction photocatalysts with high carrier separation and mobility through a thermal polymerization-hydrothermal strategy. The high concentration of photogenerated carriers facilitates the activation of oxygen and H2O2, leading to increased production of ROS (⋅O2 -, ⋅OH, h+), thereby enhancing the photocatalytic desulfurization (PODS). Additionally, DFT (Density functional theory) calculations were utilized to determine the electron migration pathways of the catalysts and adsorption energies of DBT (dibenzothiophene). Moreover, Gibbs free energy calculations indicated that MIL101/CDs-C3N4 exhibited the lowest activation energy for oxygen and H2O2. The mechanism of photocatalytic desulfurization was proposed through a combination of theoretical calculations and experimental studies. This study provides guidance for the development of MOF-based Z-scheme systems and their practical application in desulfurization processes.

Heterogeneous integration photoferroelectrics for self-powered photoelectric detectors

The anomalous photovoltaic effect inherent in ferroelectric materials brings promising opportunities for self-powered photoelectric detectors. However, the photoelectric detection performances in photoferroelectrics are limited by the low photocurrent output due to the recombination and low separation ability of photogenerated carriers. This work proposes a heterogeneous integration technology for self-powered photoelectric detectors by designing a P-type/N-type/P-type (PNP) ferroelectric junction with sandwich structure, in which not only the photogenerated carrier separation is strengthened due to the enhanced polarization derived from the interface compressive stress, but also the carrier recombination is suppressed by the built-in electric field in the depletion layer. Thus, the photocurrent output in the PNP heterojunction is increased by more than seven times at 0 V bias compared with N-type ferroelectric film and exhibits excellent responsivity and detectivity. The temperature stability for repeatable time-resolved self-powered photocurrent demonstrates applicability in high temperature environments. This work provides a feasible strategy for high-performance self-powered photoelectric detectors by heterogeneous integration in photoferroelectrics, promoting ferroelectric photonic applications.

Heterogeneous integration photoferroelectrics for self-powered photoelectric detectors

The anomalous photovoltaic effect inherent in ferroelectric materials brings promising opportunities for self-powered photoelectric detectors. However, the photoelectric detection performances in photoferroelectrics are limited by the low photocurrent output due to the recombination and low separation ability of photogenerated carriers. This work proposes a heterogeneous integration technology for self-powered photoelectric detectors by designing a P-type/N-type/P-type (PNP) ferroelectric junction with sandwich structure, in which not only the photogenerated carrier separation is strengthened due to the enhanced polarization derived from the interface compressive stress, but also the carrier recombination is suppressed by the built-in electric field in the depletion layer. Thus, the photocurrent output in the PNP heterojunction is increased by more than seven times at 0 V bias compared with N-type ferroelectric film and exhibits excellent responsivity and detectivity. The temperature stability for repeatable time-resolved self-powered photocurrent demonstrates applicability in high temperature environments. This work provides a feasible strategy for high-performance self-powered photoelectric detectors by heterogeneous integration in photoferroelectrics, promoting ferroelectric photonic applications.

Enhanced photocatalytic activity and antibacterial potential of a novel ternary ZnO-Ag2MoO4-AgI heterojunction photocatalyst

The construction of heterojunctions is a recognized strategy for enhancing photogenerated carrier separation. This research introduces a novel ZnO-Ag2MoO4-AgI photocatalyst with a double Z-type heterojunction, made using a straightforward precipitation technique. The precise position of energy levels endowed the ternary photocatalyst with the ability of directional electron flow, while the Z-type structure exhibits strong redox capabilities and facilitates the effective separation of photogenerated charge carriers. The structural characteristics, the photocatalytic activities, the antibacterial properties, and the cytotoxicity of the catalysts were evaluated. The results demonstrate that the catalytic ability of ternary composites work synergistically, surpassing the individual and binary photocatalysts. Notably, the ternary composites with 30 % AgI content exhibit the highest catalytic activity, achieving complete degradation of Rhodamine B in 30 minutes, and up to 71.2 % degradation of Norfloxacin in 60 minutes. Furthermore, more than 99.998 % of Staphylococcus aureus, and 100 % of Escherichia coli were eliminated within 40 minutes, while Human colorectal adenocarcinoma epithelial cells mortality reached 91.98 % at a dose of 250 μg/mL. Our study underscores the potential of this strategy for photocatalytic degradation of organic contaminants, and as an antibacterial agent, providing innovative insights into the design of ZnO-based heterostructure photocatalysts.

Synergistic enhancement of photocatalytic hydrogen peroxide production activity in CN/rBOB composite through double field effect

Herein, a novel rod-like bismuth bromide oxide (rBOB) was prepared by using a Bi3+ delayed-release strategy and H+ capping competition effect. And rBOB was combined with graphite carbon nitride (CN) to construct S-scheme heterojunction material (CN/rBOB). This work focused on the regulation mechanism of the rod-like morphology of rBOB and the photocatalytic H2O2 production (PHP) performance of CN/rBOB under the action of an external magnetic field. The results showed that the magnetic field can significantly increase the photocurrent response and intrinsic carrier concentration of the catalyst. And the magnetic field action improved the PHP of CN/rBOB from 1.81 to 3.31 mmol·g−1·h−1. This "internal electric field-external magnetic field" synergistic tuning obviously improves the efficiency of photogenerated carrier separation and transport to the surface active sites, which is a simple and useful strategy to construct high-quality photocatalytic systems.

Built-in electric field mediated S-scheme charge migration and Co-N4(II) sites in cobalt phthalocyanine/MIL-68(In)-NH2 heterojunction for boosting photocatalytic nitric oxide oxidation

The efficiency of photocatalytic Nitric Oxide(NO) oxidation is limited by the lack of oxygen(O2) active sites and poor charge carrier separation. To address this challenge, we developed a molecular Cobalt Phthalocyanine modified MIL-68(In)–NH2 photocatalyst with a robust Built-in electric field(BIEF). In the 2 % CoPc-MIN sample, the BIEF strength is increased by 3.54 times and 5.83 times compared to pristine CoPc and MIL-68(In)–NH2, respectively. This BIEF facilitates the efficient S-scheme charge transfer, thereby enhancing photogenerated carrier separation. Additionally, the Co-N4(II) sites in CoPc can effectively trap the separated photoexcited electrons in the S-scheme system. In addition, the Co-N4(II) sites can also serve as active sites for O2 adsorption and activation, promoting the generation of superoxide radical (O2–), thereby driving the direct conversion of NO to nitrate(NO3–). Consequently, the 2 % CoPc-MIN sample exhibits a remarkable photocatalytic NO removal efficiency of 79.37 % while effectively suppressing the formation of harmful by-product nitrogen dioxide(NO2) to below 3.5 ppb. This study provides a feasible strategy for designing high-efficiency O2 activation photocatalysts for NO oxidation.

In2S3-modified ZnIn2S4 enhanced photogenerated carrier separation efficiency and photocatalytic hydrogen evolution under visible light

ZnIn2S4 (ZIS) has limited photocatalytic hydrogen production due to low visible light utilisation and insufficient separation efficiency of photogenerated carriers. This study utilized a simple hydrothermal method to prepare In2S3/ZnIn2S4 (INS/ZIS) heterojunctions. The addition of In2S3 (INS) improves the separation and movement of photogenerated charges, and makes better use of visible light. The material was analysed using SEM, TEM, XRD, XPS and photoelectrochemical tests. Results from the transient photocurrent (TPR) and photoluminescence (PL) experiments show a photocurrent density of approximately 1.8 μA/cm2, which is 3 times greater than the ZIS (0.6 μA/cm2) density, when the INS mass is 5 %. And at this time, INS/ZIS boasts the most effective photogenerated carrier separation. The hydrogen photocatalytic generation test results showed that the photocatalytic hydrogen production rate of 5-INS/ZIS (5690 μmol/g/h) was 8.4 and 66.9 times higher than that of pure ZIS (710 μmol/g/h) and INS (89 μmol/g/h), respectively. The enhanced activity is due to the creation of type II heterojunctions, which improve the separation and transfer of light-generated charges. The research presents an innovative approach to creating composites based on ZIS.

Fabrication of ternary Bi2S3/BiVO4/g-C3N4 composite material for enhanced photocatalytic degradation of antibiotics

Antibiotic contaminants are known to pose a serious threat to the human health and environment, thus a great deal of effort has been made to develop destruction technologies for antibiotic treatment in the water environment. Photocatalytic oxidation technology is regarded as one of the most promising strategies for decomposing antibiotics from water. In this work, ternary Bi2S3/BiVO4/g-C3N4 composite material is dexterously designed and synthesized to obtain the enhanced photocatalytic performance for tetracycline (TC) degradation via a facile strategy. Therein, the optimal Bi2S3/BiVO4/g-C3N4 material showed the excellent degradation efficiency under visible light irradiation in comparison to the nude g-C3N4 and BiVO4/g-C3N4 photocatalysts, and it can continuously degrade the TC pollutant in 90 min and achieve a degradation percentage of 80.7 %. The designed materials can not only intensify photo-absorption efficiency of g-C3N4 material, but also improve its separation and transfer efficiency of photo-generated charge carriers, which is attributed to the incorporation of BiVO4 and Bi2S3 materials. The active species trapping experiments verified that the superoxide radicals (•O2−) is the main active species, and holes (h+) also played an important role in the Bi2S3/BiVO4/g-C3N4 system. Furthermore, the photoelectrochemical measurement (PEC) clearly demonstrated that the incorporation of BiVO4 and Bi2S3 materials could accelerate the separation and transfer of photo-generated electron and hole pairs. As expected, our present work could spark new inspirations to further develop the efficient photocatalysts for solar energy conversion.

Unraveling the nature of local field distortion-induced dual electron-trapping centers for efficient photocatalytic fuel evolution

Active electron-trapping centers play significant roles in photocatalysis. Herein, we synergize local field distortion and defects in nanocrystals to produce dual electron-trapping centers and unravel the nature of aluminum doping in porous ZnO with tunable amounts of heteroatoms and oxygen vacancies. The introduced Al atoms in the structural domain induce local field distortion and trigger the movement of Zn2+ from a singlet low spin state to a stable triplet state, resulting in the generation of free carriers trapping centers and optimized electronic energy band structure. Dual active electron-trapping centers of heteroatoms and oxygen vacancies promote the Separation of photo-generated charge carriers and reduce the adsorption energies of H* species. Furthermore, the d-band center of Al-doped ZnO with oxygen vacancies shifts to a higher energy position, thus promoting the adsorption and desorption of hydrogen intermediates and exhibiting 4-fold the photocatalytic H2 efficiency of pristine ZnO. This study provides new insights into the rational design of highly efficient oxide-based photocatalysts toward sustainable solar fuel evolution.

High molecular oxygen activation capacity of carbon defective g-C3N5 for photocatalytic degradation of antibiotics in water

In this study, a carbon deficient g-C3N5 for photocatalytic degradation of antibiotics in water was prepared by thermal polymerization at 600 °C followed by hydrothermal at 180 °C for 12 h, and named CN600-12. The variation of XRD patterns in the physical phase characterization combined with calculations for energy bands in density functional theory (DFT) presents a method for analyzing defects in g-C3N5. The degradation efficiency of CN600-12 on different antibiotics and dyes reached 90 % within 90 min, proving its excellent universal applicability. In addition, the prepared CN600-12 has superior stability and environmental friendliness. The burst experiments and ESR data reflect the high yields of oxygenated reactive groups (·O2– and 1O2). The oxygen adsorption capacity of the materials was calculated by combining DFT, the effect of defect configuration on oxygen adsorption was analyzed, and photoelectrochemical characterization explored their photogenerated carrier separation ability. The results show that introducing carbon defects improves the adsorption capacity of the material for oxygen. At the same time, improving the energy band structure and the separation of photogenerated carriers give the material a strong activation capacity for molecular oxygen. This study provides a feasible reference for solving the problem of antibiotic pollution in water bodies.

Z-scheme metal organic framework/Ag@AgCl heterojunction photocatalysts with elevated photocatalytic N2 fixation activity

As one of the most consumed chemical reagents, ammonia (NH3) has a wide range of applications in many fields. The demand for ammonia may continue to increase with the advancement of technology and the acceleration of industrialization. The traditional high energy consumption and high pollution ammonia synthesis methods (Haber-Bosch) need to be optimized and improved to reduce environmental pollution and energy dependence. In this work, a series of Z-scheme NM/Ag@AgCl heterojunctions were prepared as catalysts for the research of photocatalytic nitrogen fixation. By in-situ photodeposition, Ag@AgCl was uniformly distributed on the NM surface, and the interfaces of different substances were tightly bonded. The SPR effect that generated by Ag nanoparticles significantly enhanced the light energy absorption performance of heterojunction materials. In the ESR spectra, the signal peak intensity of NM/Ag@AgCl was higher than that of NM under light condition. Constructing of heterojunction was beneficial to the formation of Ti3+. The strong built-in electric field among NM and AgCl promoted the generation of Z-scheme heterojunction. NM/Ag@AgCl had sufficient redox potential to overcome thermodynamic barriers and drive the catalytic reaction. Without adding any sacrificial reagent, the ammonia production of NM/Ag@AgCl-3 reached 76.7 µmol g−1 h−1 under full spectrum radiation. The rate of ammonia formation of NM/Ag@AgCl was almost seven times than that of NM. The synergistic effect between NM and Ag@AgCl optimized the photogenerated carrier separation path. This work provided a new vision for the practical application of efficient photocatalytic N2 reduction.