Photocurrent Intensity Research Articles

A mixed valence decanuclear cerium-oxo cluster CeIII4CeIV6 for efficient photocurrent response

Cerium-oxo clusters with mixed valence exhibit distinctive redox properties due to cerium ions switch between +3/+4 valence states. However, the design and synthesis of these clusters present formidable challenges, resulting in limited availability of such species, often necessitating the use of both CeIII and CeIV reactants. Herein, we successfully obtained a mixed valence cerium-oxo cluster CeIII4CeIV6(µ3-O)4(µ4-O)4(acac)14(CH3O)6(CH3OH)2 (CeIII4CeIV6, Hacac = acetylacetone) through low-temperature crystallization only using the trivalent cerium salt. The coexistence as well as the distribution of Ce ions in different valence states have been determined from a multifaceted analysis. In addition, the stability of the synthesized cluster was confirmed by the HRESI-MS study through redissolution of the single crystal sample in fresh methanol. Importantly, Importantly, this study reveals the mechanism for the generation of +4 valence state. Under alkaline conditions, the presence of trace oxygen and the involvement of acetylacetone ligand facilitated the partial oxidation of CeIII to CeIV. The cluster CeIII4CeIV6 has strong ultraviolet absorption and long visible light absorption. As the electrode precursor, CeIII4CeIV6 showed clear photocurrent response and high photocurrent intensity due to CeIII/CeIV redox reaction.

Triggering “signal-on” photoelectrochemical responses by heterojunction transition for selective detection of copper(II) based on Pd/MoS2@g-C3N4 nanocomposites

Controlling the concentration of copper(II) in aquatic systems is of importance for human health. Numerous traditional technologies to detect Cu2+ may encounter with limitations, such as high signal background and complicated operation. Herein, a highly selective photoelectrochemical (PEC) sensor is proposed for the “signal-on” detection of Cu2+ employing g-C3N4 nanosheets with MoS2 and Pd quantum dots deposited (Pd/MoS2@g-C3N4). Pd/MoS2@g-C3N4 could present the enhanced photocurrents of specific responses to Cu2+ under light irradiation. MoS2 quantum dots on the sensor are agglomerated into MoS2 bulk during sensing Cu2+, forming an efficient Z-scheme heterojunction. The heterojunction transition induced photoelectrons transferring from the bulk MoS2 to g-C3N4, resulting in “signal-on” PEC responses. Such Z-scheme heterojunction has conquered the traditional heterojunction towards “signal-on” mechanism, that was further verified by band structure measurements and DMPO spin trapping ESR analysis. Photocurrent intensities increased gradually with the addition of incremental Cu2+ concentrations, achieving a detection limit of 0.21 μM and a broad linear interval range from 1 μM to 1 mM with high selectivity and stability. This work may open a new door towards the in situ construction of g–C3N4–based Z-scheme heterojunctions for the signal-on PEC sensing platform, providing wide applications in environmental monitoring and food safety.

Fabricating the ternary CeO2@CNTs/CdSe composite with synchronously enhanced adsorption and photocatalytic activity toward water-soluble pollutants removal

Constructing heterogeneous catalyst with different bandgaps is a prospect way to realize efficient charge transfer of catalytic redox reaction. Semiconductor-based catalyst as a prospective material can effectively solve sewage issues under light irradiation, but the efficiency is greatly influenced by the recombination rate of photoelectrons and holes. In this work, cerium dioxide (CeO2) nanoparticles (NPs) were grown in-situ on carbon nanotubes (CNTs), which can maintain the pollutant removal efficiency of pure CeO2 NPs and enhance the adsorption intensity under visible light for CeO2@CNTs composite. Furthermore, the introduction of cadmium selenide (CdSe) was conducive to establish built-in electronic field in the ternary CeO2@CNTs/CdSe catalyst, which effectively enhanced the catalytic activity of CeO2@CNTs/CdSe. In comparison to CNTs, CdSe, CeO2 and CeO2@CNTs composite, the ternary CeO2@CNTs/CdSe catalyst exhibited higher photocurrent intensity, lower recombination of photoelectrons and holes (e-/h+) pairs, indicating much better photocatalytic activity. CeO2@CNTs/CdSe as photocatalyst displayed excellent adsorption ability for Congo red (CR), which contributed to increase the transparency of reaction solution and improve the utilization rate to light, the evaluated degradation efficiency of CR achieved 83.58 % and the reduction ratio of Cr(VI) was nearly 100 %. This work confirms that CeO2@CNTs/CdSe composite with excellent adsorption and photocatalytic ability is a promising photocatalyst material in wastewater treatment.

Plasmonic-Enhanced Tunable Near-Infrared Photoresponse for Narrowband Organic Photodetectors.

Near-infrared (NIR) narrowband organic photodetectors (OPDs) can be essential building blocks for emerging applications including wireless optical communication and light detection, but further improvement of their performances remains to be a great challenge. Herein, a light manipulation strategy combining solution-processable gold nanorings (AuNRs)-based hole transporting layer (HTL) and an optical microcavity is proposed to achieve high-performance NIR narrowband OPDs. Optical microcavities with a Fabry-Pérot resonator structure, guided by theoretical simulation, are coupled with PM6:BTP-eC9-based OPDs to exhibit highly tunable NIR selectivity. The further integration of AuNRs array with NIR-customized localized surface plasmon resonance in the HTL of the NIR narrowband OPDs enables evident NIR absorption enhancement, yielding a specific detectivity exceeding 1013 Jones (1.5 × 1012 Jones, calculated from noise spectral density) at 820 nm, along with a finely selective photoresponse (full width at half-maximum of 80 nm) and a 3-fold increase in photocurrent intensity. Finally, the practical application of our OPDs is demonstrated in an NIR communication system. These results reveal the great potential of an appropriate optical design for developing highly performing NIR narrowband OPDs.

Two iodoargentate hybrids: syntheses, crystal structures, photocurrent responses and theoretical studies

In recent years, organic-inorganic hybrid iodoargentates have suffered extensive research attention due to their rich structures and unique optical and semiconductor properties. In this article, using 4,4'-dbbpy (4,4'-dbbpy = 4,4'-dibromo-2,2-bipyridine) and 5,5'-dbbpy (5,5'-dbbpy = 5,5'-dibromo-2,2-bipyridine) ligands as structural modifiers, two new iodoargentate hybrids, namely [Ni(4,4'-dbbpy)3]AgI3 (1) and [Ni(5,5'-dbbpy)3]Ag2I4 (2) have been successfully constructed, which are then structurally, optically and theoretically studied. Compounds 1 and 2 have optical band gaps at 2.45 and 2.56 eV, displaying visible light responding photocurrent intensities of 0.26 and 0.47 μA·cm−2, respectively. Additionally, the Hirshfeld surface analyses and density of states have also been investigated.

A photoelectrochemical sensor for glutathione detection without additional electron donor using CNTs/Bi4VO8Br/CdS nanocomposites

The concentration of glutathione in the human body has a significant impact on health, which highlights the increasing urgency to develop highly sensitive methods for its detection. In this study, indium tin oxide (ITO) conductive glass was used as the substrate, and CNTs/Bi4VO8Br nanocomposites and CdS were sequentially modified, which were used as sensing and recognition elements. The usage of CNTs in the electrode design provides enhanced electron transfer rates due to their excellent conductivity, which ultimately results in an increase in the photocurrent intensity. Furthermore, the sensitization effect of CdS in the nanocomposite significantly improves the photocurrent intensity of the sensing system. Utilizing the exceptional photoelectrochemical properties of the aforementioned materials, a highly sensitive photoelectrochemical sensor has been developed for the detection of glutathione. The sensor effectively detects glutathione in the concentration range of 5–1000 μmol/L, with a detection limit of 0.67 μmol/L (S/N = 3). Additionally, the constructed sensor exhibits excellent stability, specificity, and reproducibility.

Facile fabrication of low-defect spinel zinc ferrite oxide thin film for high-performance ultraviolet photodetector

ZnFe2O4 (ZFO) has gained much attention for numerous applications such as photocatalysis and lithium-ion batteries owing to its unique magnetic, optical, and electrical properties, low toxicity, and high chemical stability. However, current research on this material for the development of solid-state photodetectors is insufficient. For the first time, a high-purity and compact ZFO thin film was prepared via a simple sol-gel method and used as an efficient n-type photoactive material for ultraviolet A (UVA) detection. When ZFO is coupled with a p-type polymer, the high-quality p-n heterojunction can be used as a self-powered UV detector with a high on/off ratio of > 103, excellent detectivity of 3 × 1011 Jones, and a linear relationship between the photocurrent and light intensity. Accordingly, this study suggests that the novel ZFO-based photodiode prepared via a facile process could be industrially scalable and employed in practical UV detection applications.

X-ray Spectroscopy of a Rare-Earth Molecular System Measured at the Single Atom Limit at Room Temperature.

We investigate the limit of X-ray detection at room temperature on rare-earth molecular films using lanthanum and a pyridine-based dicarboxamide organic linker as a model system. Synchrotron X-ray scanning tunneling microscopy is used to probe the molecules with different coverages on a HOPG substrate. X-ray-induced photocurrent intensities are measured as a function of molecular coverage on the sample, allowing a correlation of the amount of La ions with the photocurrent signal strength. X-ray absorption spectroscopy shows cogent M4,5 absorption edges of the lanthanum ion originated by the transitions from the 3d3/2 and 3d5/2 to 4f orbitals. X-ray absorption spectra measured in the tunneling regime further reveal an X-ray excited tunneling current produced at the M4,5 absorption edge of the La ion down to the ultimate atomic limit at room temperature.

N-doped carbon quantum dots enhance anaerobic digestion under light condition: The performances and potential mechanisms

The treatment of organic waste (OW) by anaerobic digestion (AD) conforms to the concept of sustainable development. But AD is facing the issue of low conversion rate. In this work, the photo-AD system using visible light (LED lamp) as the source was constructed and the performances and mechanism of N-doped carbon quantum dots (NCQD) were explored in the system for the first time. The results showed that 0.5 g/L NCQD promoted a 23.1 % increase in cumulative CH4 yield in the photo-AD system. Microbial analysis results showed that in photo-AD with NCQD, the dominant strain was Methanosarciniales, with an abundance of 69.0 %. Microbial activity and structural integrity tests showed that the microorganisms were not damaged by free radicals. In addition, NCQD increased the redox peak intensity of the CV curve and increased photocurrent intensity of photo-AD. Furthermore, it promoted an increase of 18.2 % (0.26 ± 0.03 μmol/mL) in ATP concentration. The photoelectrochemical analysis and quantitative analysis of functional genes results indicated that NCQD mainly promoted methanogenesis by providing photoelectrons. This promotion mechanism increased the copynumber (61,652.8 g−1) of EchA in photo-AD, rather than Vht and Hdr related to cytochrome. This work provided new strategies for the enhancement of AD and clarified potential mechanisms.

A “turn-on” photoelectrochemical DNA biosensor based on charge transfer between BiVO4 and gold nanoparticles

An enhanced charge transfer between BiVO4 and Au nanoparticles (AuNPs) was utilized to design a “turn-on” photoelectrochemical (PEC) biosensor for sensitive detection of target DNA. The calcination of BiVO4 on indium tin oxide (ITO) substrate was integrated with Au nanoparticles (NPs) labelled probe DNA (pDNA-AuNPs) as photoelectrode (ITO/BiVO4/pDNA-AuNPs). The cathodic photocurrent increased due to the coupling BiVO4 with AuNPs, which acted as the blank signal of this PEC platform. The probe specifically recognized and captured the target DNA (tDNA) to form double strain DNA (dsDNA) after hybridization. The photocurrent intensity of the ITO/BiVO4/dsDNA-AuNPs photoelectrode further increased due to the enhancement of the charge transfer between BiVO4 and AuNPs through dsDNA chain. This photocurrent enhancement was linear proportional to the logarithm of tDNA concentration. Based on this strategy, the PEC assay displayed a linear range from 1 aM to 10 pM and the detection limit was as low as 0.2 aM (S/N = 3). It provides a promising platform for ultrasensitive target DNA detection, and thus shows a great potential in genetic disease or cancer diagnostics and infectious pathogen detection.

Solvothermal syntheses and characterization of one-dimensional (1,4-dabH2)Cu1.72Ag0.28SnSe4 (1) and (1,4-dabH2)Cu2SnSe4 (2)

Here, two seleniumstannates (1,4-dabH2)Cu1.72Ag0.28SnSe4 (1) and (1,4-dabH2)Cu2SnSe4 (2) (1,4-dab = 1,4-diaminobutane), were synthesized successfully via solvothermal method, and an organic amine as the structural directing agent. Two compounds have similar structures: inorganic anionic chains and doubly protonated [1,4-dabH2]2+ organic cations. In this work, single-crystal and powder X-ray diffraction and thermogravimetric-differential thermal analysis (TG-DTA) are used to verify the above compounds, meanwhile, the optical and photoelectric properties were investigated, and the optical band gap is calculated as 2.43 and 2.46 eV, respectively. Furthermore, 1 and 2 exhibited photocurrent responses with photocurrent intensities of 3.83 μA/cm2 and 1.54 μA/cm2, respectively. Additionally, the compounds degrade methylene blue (MB).

Facile preparation of In2O3–In2S3 core–shell composites for the enhanced photoelectric activity

AbstractThis study examines In2S3 concentration to the photo‐induced current density of particulate In2O3–In2S3 composite heterostructures under visible light irradiation. A self‐templated approach involving hydrothermal sulfidation of In2O3 nanofibers with thioacetamide (TAA) in water produces the In2O3–In2S3 core–shell structure at a moderate temperature. The In2S3 fraction is readily tunable by adjusting the TAA concentration. Incorporating In2S3 (45–82 wt.%) leads to a decreased bandgap from 3.1 to ca. 2.3 eV, enabling the harvest of partial visible‐light energy to create charged carriers efficiently. The photocurrent is particularly pronounced when the In2O3–In2S3 composites consist of 45 wt.% In2S3, to which the photocurrent intensity is more significant than 0.1 mA⋅cm−2 at 0.8 V in 0.1 M Na2SO4 solution compared to less than 0.01 mA⋅cm−2 for the rest of the In2O3–In2S3 counterparts. This is attributable to the enhanced electron–hole separation at the semiconducting heterojunction and the more efficient use of the light spectrum due to the narrowing bandgap.

DNAzyme-Mediated Biodeposition Coupling Adjustable Cascade Electric Fields for Photoelectrochemical Telomerase Activity Monitoring.

Telomerase, as a specialized reverse transcriptase, plays a vital role in early cancer diagnostics and prognosis; thus, developing efficient sensing technologies is of vital importance. Herein, an innovative "signal-on-off" photoelectrochemical (PEC) sensing platform was developed for ultrasensitive evaluation of telomerase activity based on an electron-transfer tunneling distance regulation strategy and DNAzyme-triggerable biocatalytic precipitation. Concretely, cascade internal electric fields between CuInS2 quantum dots (QDs), graphitic carbon nitride nanosheets (g-C3N4 NSs), and TiO2 nanorod arrays (NRAs) were developed to realize cascade electron extraction and hole transfer. Enabled by such a design, an effective "signal-on" state to gain a progressively enhanced PEC output was designed by suppressing the photogenerated electron-hole pair recombination. With the introduction of hairpin probe H2 and the subsequent extension of the primer sequence driven by the target telomerase, the CuInS2 QDs labeled with hairpin probe H1 were programmatically unfolded, resulting in CuInS2 QDs' close proximity to the working electrode away from the cascade interface, accompanied by the formation of G-quadruplex/hemin complexes. The gradual undermining of tunneling distance and implantation of DNAzyme-initiating biocatalytic precipitation tremendously induced the sluggish migration kinetics of the photoinduced charge, accompanied by the photocurrent intensity decrement, leading to the "signal-off" state. Under optimized conditions, the as-prepared PEC biosensor realizes ultrasensitive detection of telomerase activity from 10 to 105 cell·mL-1 with a detection limitation of 3 cells·mL-1. As a proof of concept, this well-designed method provides new insights into signal amplification for telomerase activity evaluation and also presents promising potential for further development in drug screening, healthcare diagnostics, and biological assays.

Multipath collaboration mechanisms involved in the photocatalytic reduction of Cr(VI) by FeC2O4/Bi2.15WO6

FeC2O4/Bi2.15WO6 (FeC2O4/BWO) composites were prepared, and the mechanism involved in the photocatalytic reduction of Cr(VI) by FeC2O4/BWO was investigated. When the doping amount of FeC2O4 was 10%, the obtained 10-FeC2O4/BWO composite exhibited the best Cr(VI) reduction activity with a rate constant of 0.1934 min−1, which was 33.3 times higher than that of BWO. The improved photocatalytic performance of 10-FeC2O4/BWO was ascribed to the efficient carrier separation, which was confirmed by the higher transient photocurrent and lower PL intensity than single BWO. Capture experiments further revealed that photogenerated electrons were the major species for reducing Cr(VI) by 10-FeC2O4/BWO. Dissolved Fe(II) (Fe(II)diss) released from the surface of FeC2O4 can reduce Cr(VI) to Cr(III) directly, along with the formation of Fe(III)diss. Meanwhile, the potential difference between BWO and FeC2O4 can form a built-in electric field. This field facilitates the movement of photogenerated electrons, leading to the conversion of Fe(III)diss to Fe(II)diss, could transform and drive the circulation of ‘Fe(II)diss-Fe(III)diss-Fe(II)diss’. Furthermore, the electrons transferred to the conduction band (CB) of BWO enhance the reduction of Cr(VI). The above multipath collaboration mechanism enhanced the reduction of Cr(VI) by 10-FeC2O4/BWO. Therefore, this study provides data basis and theoretical support for remove Cr(VI) and other pollutants.

Synthesis of Ag3PO4/Ag/g-C3N4 Composite for Enhanced Photocatalytic Degradation of Methyl Orange.

In this study, we have successfully constructed Ag3PO4/Ag/g-C3N4 heterojunctions via the hydrothermal method, which displays a wide photo-absorption range. The higher photocurrent intensity of Ag3PO4/Ag/g-C3N4 indicates that the separation efficiency of the photogenerated electron-hole pairs is higher than that of both Ag3PO4 and Ag/g-C3N4 pure substances. It is confirmed that the efficient separation of photogenerated electron-hole pairs is attributed to the heterojunction of the material. Under visible light irradiation, Ag3PO4/Ag/g-C3N4-1.6 can remove MO (~90%) at a higher rate than Ag3PO4 or Ag/g-C3N4. Its degradation rate is 0.04126 min-1, which is 4.23 and 6.53 times that of Ag/g-C3N4 and Ag3PO4, respectively. After five cycles of testing, the Ag3PO4/Ag/g-C3N4 photocatalyst still maintained high photocatalytic activity. The excellent photocatalysis of Ag3PO4/Ag/g-C3N4-1.6 under ultraviolet-visible light is due to the efficient separation of photogenerated carriers brought about by the construction of the Ag3PO4/Ag/g-C3N4 heterostructure. Additionally, Ag3PO4/Ag/g-C3N4 specimens can be easily recycled with high stability. The effects of hydroxyl and superoxide radicals on the degradation process of organic compounds were studied using electron paramagnetic resonance spectroscopy and radical quenching experiments. Therefore, the Ag3PO4/Ag/g-C3N4 composite can be used as an efficient and recyclable UV-vis spectrum-driven photocatalyst for the purification of organic pollutants.

Constructed CdS/Mn-MOF heterostructure for promoting photocatalytic degradation of Rhodamine B

A new 3D Mn-MOF was prepared with the ligand H2L (H2L = 5-(pyrazin-2-yl) isophthalic acid) by solvothermal method. Then the Mn-MOF was used as a precursor to synthesize CdS/Mn-MOF composites. The degradation efficiency of Rhodamine B (RhB) by CdS/Mn-MOF (theoretical mass ratio of CdS to Mn-MOF is 1:1) is 98.7% in 60 min, which is 19.7 times and 2.3 times that of Mn-MOF and CdS, respectively. The outstanding performance is owed to the loading of CdS, which significantly broadens the photoresponsive range of Mn-MOF and improves the utilization of visible light. Meanwhile, the heterojunction formed between Mn-MOF and CdS can effectively inhibit the recombination of photogenerated electrons and holes. Furthermore, the photocurrent intensity of CdS/Mn-MOF(50) is higher than that of Mn-MOF and CdS. The photocatalytic performance of CdS/Mn-MOF(50) also exhibits excellent stability and reusability. In addition, the enhanced mechanism of photocatalytic activity was investigated systematically.

Ultra-sensitive photoelectrochemical biosensor for determination of African swine fever virus based on surface plasmon resonance

Sensitive and specific detection of African swine fever virus (ASFV) is crucial for agricultural production and economic development due to the mortality and infectivity. In this study, a bismuth induced enhanced photoelectrochemical (PEC) biosensor based on in-situ loop mediated isothermal amplification (LAMP) was constructed using deposited bismuth nanoparticles loaded bismuth oxycarbonate (Bi/(BiO)2CO3) as photoactive material, using primers designed according to LAMP as recognition elements, and using in-situ LAMP to achieve nucleic acid amplification of target genes. As the Bi induced surface plasmon resonance (SPR) effect, enhanced light captures and effective electron hole separation, it could effectively enhance the photoelectric activity, so the prepared Bi/(BiO)2CO3 nanohybrid had higher photocurrent intensity and good stability. The constructed PEC biosensor has realized the detection of ASFV in real samples with good sensitivity, specificity and repeatability. In the range from 1.0 × 10−13 to 1.0 × 10−7 g/L, the photoelectric current decreased with the increase of the concentration of ASFV, and the detection limit was 3.0 × 10−14 g/L (about 0.048 copies/μL). Combining the advantages of LAMP with the excellent performance of PEC, it provides a simple, economical and efficient method for nucleic acid diagnosis, and also provides a new idea for biosensor detection.

Bi2WO6@g-C3N4 Heterostructure for Cathodic Photoelectrochemical Dopamine Sensor

A simple and low-cost cathodic photoelectrochemical (PEC) sensor based on Bi2WO6@g-C3N4 was designed for dopamine (DA) detection. The Bi2WO6 nanoflower was first prepared using a simple hydrothermal method followed by the combination with g-C3N4 nanosheet to form the Bi2WO6@g-C3N4 heterostructure. The heterostructure can extend the absorbance to the visible region and accelerate the transfer of charge carriers. Furthermore, DA easily coordinates with exposed Bi3+ on the Bi2WO6 surface and forms the charge-transfer complex to further enhance the cathodic photocurrent. Under optimal conditions, there are two linear relationships between the concentration of DA and photocurrent intensity. The linear ranges are 0.1–10 µM and 10–250 µM, with a sensitive detection limit (LOD) of 28 nM. Notably, the real sample of human blood serum analysis further revealed the accuracy and feasibility of the Bi2WO6@g-C3N4-based PEC platform. Convincingly, the heterostructure of Bi2WO6 and g-C3N4 opened up a new avenue for the construction of DA analysis.

Porphyrin and molecularly imprinted polymer double sensitized cathode photoelectrochemical sensor for chlortetracycline

A molecularly imprinted photoelectrochemical (PEC) sensor was fabricated for the detection of chlortetracycline (CTC) based on 5,10,15,20-tetrakis(4-carboxylphenyl) porphyrin (TCPP) and poly(o-phenylenediamine) (PoPD) sensitized ZnO-MWCNTs-NH2, which was prepared by a three-steps synthetic route: a simple one-step hydrothermal method for ZnO-MWCNTs-NH2, a successive self-assembly for TCPP loading and in situ electro-polymerization for multifunctional PoPD. Here MWCNTs-NH2 was introduced not only to narrow the band gap of ZnO for enhance visible light absorption, but also to upgrade the surface property for TCPP and PoPD loading, which improved the photocurrent of the photoactive electrode greatly. Besides good selectivity, PoPD film exhibited well energy level matching with ZnO-MWCNTs-NH2/TCPP, thus benefiting for the formation of heterojunction and the separation and transmission of photogenerated carriers. Based on the good matching of organic and inorganic components, a novel cathode MIP-PEC sensor for CTC with good sensitivity and selectivity was constructed. Under the optimized conditions, the MIP-PEC sensor possessed a good linear relationship between the photocurrent intensity and concentration of CTC from 0.5 nmol/L to 10 μmol/L with a detection limit of 0.17 nmol/L (S/N = 3). And it could be used for the detection of CTC in actual samples (e.g. lake water, milk and pork) with recoveries among 86.4%–112.0%, indicating its good practicality.

Adsorption-enhanced photocatalytic waterborne virus inactivation by graphite carbon nitride conjugated with covalent organic frameworks

The increasing outbreaks of virus-related diseases drive the need to inactivate waterborne viruses efficiently and eco-friendly. Here, g-C3N4@COF heterojunction photocatalysts were synthesized for adsorption-enhanced photocatalytic inactivation of viral surrogates (phage MS2). The modified g-C3N4 outperformed g-C3N4 nanosheets in charge-carrier separation and quantum yield (with photocurrent intensity of 0.15 vs 0.02 μA and fluorescence lifetime of 11.6 vs 1.7 ns). COF exhibited a larger specific surface area (90.883 vs 20.801 m2/g) and less negative-charged surface (−13.8 vs −30.1 mV) than g-C3N4. Accordingly, modified g-C3N4 facilitated virus adsorption and improved the reactive species utilization efficiency, resulting in 7.36 times more efficient virus inactivation relative to g-C3N4. For g-C3N4@COF, the predominant reactive species causing virus inactivation through capsid destruction and genome degradation were superoxide radicals (•O2−) and photogenerated holes (h+). Interestingly, our study found the efficiency trade-offs that the appropriate adsorption of phage MS2 enhanced photocatalytic inactivation but over-adsorption affected the inactivation rate negatively. Overall, our study demonstrates that g-C3N4@COF heterojunction photocatalyst can simultaneously improve reactive species (RS) generation and utilization, which enhances the photocatalytic inactivation of waterborne viruses.