Full Solar Spectrum Research Articles

Dual Charge Transfer Generated from Stable Mixed-Valence Radical Crystals for Boosting Solar-to-Thermal Conversion.

Realizing dual charge transfer (CT) based on stable organic radicals in one system is a long-sought goal, however, remains challenging. In this work, a stable mixed-valence radical crystal is designed via a surfactant-assisted method, namely TTF-(TTF+• )2 -RC (where TTF = tetrathiafulvalene), containing dual CT interactions. The solubilization of surfactants enables successful co-crystallization of mixed-valence TTF molecules with different polarity in aqueous solutions. Short intermolecular distances between adjacent TTF moieties within TTF-(TTF+• )2 -RC facilitate both inter-valence CT (IVCT) between neutral TTF and TTF+• , and inter-radical CT (IRCT) between two TTF+• in radical π-dimer, which are confirmed by single-crystal X-ray diffraction, solid-state absorption, electron spin resonance measurements, and DFT calculations. Moreover, TTF-(TTF+• )2 -RC reveals an open-shell singlet diradical ground state with the antiferromagnetic coupling of 2J = -657 cm-1 and an unprecedented temperature-dependent magnetic property, manifesting the main monoradical characters of IVCT at 113-203 K while the spin-spin interactions in radical dimers of IRCT are predominant at 263-353 K. Notably, dual CT characters endow TTF-(TTF+• )2 -RC with strong light absorption over the full solar spectrum and outstanding stability. As a result, TTF-(TTF+• )2 -RC exhibits significantly enhanced photothermal property, an increase of 46.6°C within 180 s upon one-sun illumination.

Synergetic effect of the interface electric field and the plasmon electromagnetic field in Au-Ag alloy mediated Z-type heterostructure for photocatalytic hydrogen production and CO2 reduction

The challenge of synergistically optimizing different mechanisms limits the further improvement of plasmon-mediated photocatalytic activities. In this work, the CdS/Au-Ag/B-TiO2 photocatalyst, combining a heterojunction structure with localized surface plasmon resonance (LSPR), is prepared by a high-temperature hydrogen reduction and hot solvent method. The novel synergistic interaction at the interface between the electric field and the plasmon electromagnetic field drives effective charge separation with improved photocatalytic efficiency. The Cd3Ti2 catalyst exhibits the highest photocatalytic activity, and the H2 generation efficiency under the full solar spectrum is 15.97 mmol⋅h−1⋅g−1 with good stability as high as 81.3% in 24 h cycles. The CH4 and CO precipitation performances are achieved at 14.2 μmol⋅h−1⋅g−1 and 113.9 μmol⋅h−1⋅g−1, respectively, in the CO2RR process. The design of the synergistic mechanism of the dual electric field offers an important development in the field of plasma-mediated photoredox catalysis.

Multi-scale multi-physic coupled investigation on the matching and trade-off of conversion and storage of optical, thermal, electrical, and chemical energy in a hybrid system based on a novel full solar spectrum utilization strategy

In order to achieve a reasonable utilization of the full solar spectrum at low-cost, a photovoltaic/thermoelectric/electrolysis (PTE) hybrid system based on a novel full solar spectrum utilization strategy is proposed. The PTE mainly consist of a thermal collector with the spectrally selectively absorption fluid (water), a photovoltaic-thermoelectric (PV–TE) component and a water electrolysis component. Based the structure of the PTE, the full solar spectrum energy can be reasonably and efficiently allocated and utilized. For the complicated coupling physical process in PTE hybrid system, an integrated multi-scale multi-physic theoretical model is developed to optimize and investigate the PTE hybrid system. After the analyses on the multis-scale multi-physic effect of the air insulation layer between the thermal collector and the PV–TE component, it is found that removing air insulation layer leads to the less reflection loss and parasitic absorption, and more the maximum achievable photo current density and the internal heat source for TE component. Moreover, not only does the PV–TE component without the air insulation layer have higher efficiency (27.03%), but the concentration corresponding to the maximum efficiency increase to 31 from 3, which means more output power. By matching the structure and energy between components, the efficiency of the PTE hybrid system can be further improved, while the efficiency and energy storage of the PTE hybrid system can be adjusted according to the demand. Compared to single PV system, the efficiency of the PTE hybrid system has been increased by 15.38% at the concentration of 20, and this difference increases with the concentration. Moreover, the PTE hybrid system can simultaneously generate 200 W/m2 of hydrogen energy at the concentration of 20. In summary, the PTE hybrid system not only offers better performance (generation and storage), but also better integration, providing a guiding idea for the full solar spectrum utilization. Moreover, the multi-scale multi-physic coupled model also provides precise theoretical guidance for the optimization and design.

Super-Photothermal Effect-Mediated Fast Reaction Kinetic in S-Scheme Organic/Inorganic Heterojunction Hollow Spheres Toward Optimized Photocatalytic Performance.

Using full solar spectrum for energy conversion and environmental remediation is a major challenge, and solar-driven photothermal chemistry is a promising route to achieve this goal. Herein, this work reports a photothermal nano-constrained reactor based on hollow structured g-C3 N4 @ZnIn2 S4 core-shell S-scheme heterojunction, where the synergistic effect of super-photothermal effect and S-scheme heterostructure significantly improve the photocatalytic performance of g-C3 N4 . The formation mechanism of g-C3 N4 @ZnIn2 S4 is predicted in advance by theoretical calculations and advanced techniques, and the super-photothermal effect of g-C3 N4 @ZnIn2 S4 and its contribution to the near-field chemical reaction is confirmed by numerical simulations and infrared thermography. Consequently, the photocatalytic degradation rate of g-C3 N4 @ZnIn2 S4 for tetracycline hydrochloride is 99.3%, and the photocatalytic hydrogen production is up to 4075.65µmol h-1 g-1 , which are 6.94 and 30.87 times those of pure g-C3 N4 , respectively. The combination of S-scheme heterojunction and thermal synergism provides a promising insight for the design of an efficient photocatalytic reaction platform.

Enhanced Photocatalytic Properties of Restacked Unilamellar [SrTa2O7]2- Nanosheets of Aurivillius Phase Layered Perovskites.

In the present work, unilamellar [SrTa2O7]2- perovskite nanosheets with variable lateral dimensions were synthesized via a high-yield, three-step liquid exfoliation route from layered Bi2SrTa2O9. The photocatalytic activity of the parent and exfoliated layered perovskites was evaluated for the photocatalytic dye degradation of Rhodamine B under UV light (254 nm) and reduction of water to H2 under the full solar spectrum. A comparative study of the photocatalytic behavior of unilamellar [SrTa2O7]2- perovskite nanosheets and parent layered structure showed a significant improvement in both hydrogen evolution (98.20 vs 3 μmol g-1) and Rhodamine B degradation time (180 vs 30 min), with the restacked nanosheets. The exfoliation of layered perovskites not only increases their specific surface area, providing more active sites, but also reduces the recombination probability of electrons and holes due to their unilamellar structure and reduced charge transport pathways. The synthesis and preparation of strong acid solids such as [SrTa2O7]2- perovskite nanosheets can be a promising approach for effective adsorption of pollutants with cationic nature and more efficient electron transfer between the dye and catalyst. Finally, the photocatalytic characteristics of the restacked unilamellar [SrTa2O7]2- nanosheets remained unchanged after three successive cycles of recycling-reusing.

Enhanced carrier separation in g-C3N4/MoO3-x heterostructures towards efficient phenol removal

Two-dimensional (2D)/2D g-C3N4/MoO3-x heterojunctions were constructed for enhanced photocatalytic phenol removal. The oxygen vacancies in MoO3-x help to extend absorption in a full solar spectrum especially in near-infrared (NIR) region. Improved charge transfer path preserved photogenerated electrons and holes with powerful enough redox abilities, which simultaneously improved phenol photodegradation performance and photocatalytic activation efficiency of peroxydisulfate (PDS). In full solar spectrum activated PDS system, the phenol removal efficiency using g-C3N4/MoO3-x heterostructures reached 98% within 60 min. For the contribution of PDS activation process, active species trapping experiment and in-situ open-circuit potentials (OCP) measurement indicated that radical and non-radical pathways jointly promoted the elimination of phenol. The existence of oxygen vacancies promoted the formation of catalyst-PDS* complex and thus facilitated the electron transfer process, which exerted crucial effect as non-radical pathway. This result provided an ideal catalyst for photocatalytic persulfate activation system in the field of environmental remediation.

Turning dead leaves into an active multifunctional material as evaporator, photocatalyst, and bioplastic

Large numbers of leaves fall on the earth each autumn. The current treatments of dead leaves mainly involve completely destroying the biocomponents, which causes considerable energy consumption and environmental issues. It remains a challenge to convert waste leaves into useful materials without breaking down their biocomponents. Here, we turn red maple dead leaves into an active three-component multifunctional material by exploiting the role of whewellite biomineral for binding lignin and cellulose. Owing to its intense optical absorption spanning the full solar spectrum and the heterogeneous architecture for effective charge separation, films of this material show high performance in solar water evaporation, photocatalytic hydrogen production, and photocatalytic degradation of antibiotics. Furthermore, it also acts as a bioplastic with high mechanical strength, high-temperature tolerance, and biodegradable features. These findings pave the way for the efficient utilization of waste biomass and innovations of advanced materials.

Constructing Bi2MoO6/Pomelo-Peel-Derived Carbon 0D/3D Heterojunctions To Enhance Photothermal Catalytic CO2 Reduction in Full Solar Spectrum

The carrier migration limitation has been a key factor restricting the photothermal catalytic CO2 reduction. To further enhance carrier transport, Bi2MoO6 quantum dots (BM QDs) are deposited on the surface of alkali-activated pomelo-peel-derived carbon (CPP-A) to construct CPP-A/BM QDs 0D/3D heterojunctions in this paper. BM QDs have extremely short carrier transport distances and achieve photothermal synergy through the graded utilization of the full solar spectrum. The carbon framework of CPP promotes the high dispersion of BM QDs (3 nm) and allows the local surface temperature of the catalyst to increase rapidly up to 100 °C. The critical role of heat enhances the diffusion, adsorption, and carrier migration processes of CO2 and provides the energy to cross the CO2 activation energy barrier. More importantly, the oxygen-containing groups of CPP and BM QDs form a C–O–Bi interfacial electron bridge, which provides a high-speed channel for carrier transport across the interface, allowing many electrons generated by BM QDs to migrate rapidly to the CPP surface, inducing CPP as a new electron-rich surface for rapid CO2 activation, which results in an ultrahigh CO yield of 61.44 μmol/(g·h) for CPP-A/BM QDs, and the catalytic activity is increased by 9.12 times.

Heterojunction nanoarchitectonics of WOx/Au-g-C3N4 with efficient photogenerated carrier separation and transfer toward improved NO and benzene conversion

Topics on effectively improving the photochemical CO2/benzene/NO oxidation conversion performances of g-C3N4 based materials via charge transfer and separation enhancement are still considered challenging, despite the growing popularity of applying these materials in a variety of energy conversion related applications. Based on the idea of nanoarchitectonics, a post-nanotechnology concept, WOx/Au-g-C3N4 heterostructures are synthesized using two-step thermal polymerization and solvothermal treatment methods in this paper. Small Au nanoparticles are incorporated in superior thin g-C3N4 via mechano-chemical pre-reaction and two-step thermal polymerization (treated at 500 and 700 °C). Enhanced photocurrent density is observed after incorporation of Au, which is also in good agreement with the photocatalytic activity (H2 generation and CO2 reduction) data. Layered WOx with abundant oxygen vacancies are further incorporated into Au-modified g-C3N4 nanosheets to form heterojunctions possessing excellent photocatalytic CO2 photo-reduction performances with CO and CH4 generation rate of 5.64 and 2.58 μmolg−1h−1, respectively, under full solar spectrum. The heterojunctions constructed via in-situ formation show direct Z-scheme charge transfer pathway with improved charge separation and transport efficiencies. These highly stable and recyclable hierarchical g-C3N4 hybrid nanostructures (WOx/Au-g-C3N4 heterojunctions) show outstanding conversion rate (88.1%) and selectivity (99.3%) for benzene to phenol conversion under full solar spectrum condition, as well as excellent NO removal rate (61%).

Unveiling the latent reactivity of imines on pyridine-functionalized covalent organic frameworks for H2O2 photosynthesis

Unveiling the active site for the oxygen reduction reaction (ORR) holds the key to understanding and improving the photocatalytic activity of covalent organic frameworks (COFs) for H2O2 evolution. However, for imine-linked COFs, the role of the imine group is often overlooked in photosynthesis compared with other groups with electrophilicity or light-harvesting capabilities. Herein, a strategy is presented for eliciting the latent photoreactivity of imines by introducing an electron-acceptor structure (pyridine unit) near the imine bonds to enhance the kinetic and thermodynamic advantages of imines for the photocatalytic ORR to H2O2. Experiments and theoretical simulations indicate that the hindered visible light absorption and charge carrier separation caused by the weak electron delocalization can be substantially improved by introducing pyridinic N, leading to full solar spectrum absorption. Meanwhile, the pyridinic N can act with the N atom of the imine as an enhanced site for O2 adsorption and activation, and the strong electron transfers from COFs to O2 and ORR intermediates enable a two-step single-electron reduction route of O2 in pyridine-functionalized COFs for a more feasible H2O2 generation (706.2 µmol g−1 h−1) than original imine-linked COF (372.7 µmol g−1 h−1) under visible light irradiation. This work provides a new idea for designing and modifying imine-linked COFs in advanced photocatalytic applications.

Harnessing of low-energy IR photons via oxygen-vacancies in SrTiO3 nanocrystals for photocatalytic hydrogen production

The surface-oxygen vacancies were generated to enhance the near-IR light response of the SrTiO3 photocatalyst by heating SrTiO3 in a highly reducing environment. The UV–visible diffuse reflectance spectra of SrTiO3-Ov revealed strong absorption between 400 and 800 nm, while IPCE response was extended beyond 800 nm, confirming the near-IR light response of SrTiO3-Ov. The hydrogen production rates for SrTiO3-Ov at pH 3.0 under full solar spectrum, visible and IR radiation were 100, 25 and 10 μlg−1h−1, respectively. The respective normalized hydrogen with respect to light intensity were found to be 100, 50 and 33 μlg−1h−1 while hydrogen production of pristine SrTiO3 was less than 2 μlg−1h−1 under full solar spectrum. The mid-gap Ov and Ti3+ states in SrTiO3-Ov are key factors in the origin of the near-IR responses of the catalyst and the feasibility of using low-photonic-energy IR light to produce hydrogen by water splitting was demonstrated.

Substitution and oxygen vacancy double defects on Bi2MoO6 induced efficient conversion of CO2 and highly selective production of CH4

A series of novel iodine substitution and oxygen vacancy double defects Bi2MoO6 nanosheets for enhanced photocatalytic reduction of CO2 is reported, which exhibited superior CO2 photocatalytic activity and CH4 selectivity under full solar spectrum illumination. Bi2MoO6-I2 (the molar ratio of I to Mo is 0.13) has the highest photocatalytic activity, its CO yield is 2.0 times that of pure Bi2MoO6, the CH4 yield is 12.2 times that of pure Bi2MoO6, and the CH4 selectivity reaches 5.3 times that of pure Bi2MoO6. Its structure and physicochemical properties were investigated by material characterizations, photoelectrochemical tests and DFT calculations. The enhancement in CO2 conversion and CH4 selectivity benefit from: (1) Larger specific surface areas and smaller nanosheets thicknesses facilitate carrier migration; (2) More suitable band structure promotes the reduction of CO2; (3) Insertion of impurity energy levels in the band gap enables efficient jumping of photogenerated electrons; (4) Double defects contribute to efficient CO2 adsorption and activation; (5) Promoting highly selective conversion of CO2 to CH4 by optimising the formation energy of reaction intermediates.

Reactive Magnetron Sputtering of Large‐Scale 3D Aluminum‐Based Plasmonic Nanostructure for Both Light‐Induced Thermal Imaging and Photo‐Thermoelectric Conversion

AbstractPlasmonic nanostructures have attracted tremendous interest due to their special capability to trap light, which is of great significance for many applications such as solar steam generation and desalination, electric power generation, photodetection, sensing, catalysis, cancer therapy, and photoacoustic imaging. However, the noble metal‐based (Au, Ag, Pd) plasmonic nanostructures with expensive costs and limitations to large‐scale fabrication restrict their practical applications. Here, a novel and noble‐metal‐free Al/AlN plasmonic nanostructure fabricated by a reactive magnetron sputtering at the elevated temperature of 200 °C is presented. The unique 3D Al/AlN plasmonic nanostructures show a highly efficient (96.8%) and broadband (full solar spectrum) absorption and a strong photothermal conversion effect on its surface, demonstrating the potential in applications in light‐induced thermal imaging and photo‐thermoelectric power generation. This simple fabrication method and the developed Al/AlN plasmonic nanostructure combine excellent light trapping performance, abundant and low‐cost Al and N elements, good heat localization effect, and scalable fabrication method, suggesting a promising alternative to noble‐metal plasmonic nanostructures for photonic applications.

Enhanced interfacial charge transfer and photothermal effect via in-situ construction of atom co-sharing Bi plasmonic/Bi4O5Br2 nanosheet heterojunction towards improved full-spectrum photocatalysis

Constructing a plasmonic heterojunction photocatalyst is a prospective approach to improve full-spectrum photocatalytic performance. However, low interfacial charge transfer efficiency due to lattice mismatch severely limits its photocatalytic performance. Herein, a Bi atom co-sharing Bi/Bi4O5Br2 plasmonic heterojunctions were fabricated via in-situ reduction. Experimental characterizations and theoretical calculations demonstrate that the co-sharing Bi atom enables intimate contact in the heterointerface, significantly promoting interfacial charge transfer and separation. In addition, Bi metal's surface plasmon resonance effect extends the photoresponse to the near-infrared region and enhances the photothermal performances, significantly improving solar energy's utilization efficiency. By these prominent features, the optimized Bi/Bi4O5Br2 heterojunctions show that the photocatalytic degradation ratio of BPA reaches 100 % within 40 min under full-spectrum irradiation, which is about three times higher than that of Bi4O5Br2. Moreover, the photocatalytic efficiency was significantly increased by 7.5 times with the increase in temperature under NIR light irradiation due to the photothermal effect. This work offers new insights into the rational design of low-cost, highly efficient, and stable Bi-based plasmonic heterojunction photocatalysts for full solar spectrum utilization by integrating plasmonic nanostructures and photothermal effect.

Construction of full solar-spectrum available S-scheme heterojunction for boosted photothermal-assisted photocatalytic H2 production

The development of photocatalysts that maximize the use of solar spectra for photocatalysis for obtaining more efficient photocatalysts is urgently needed. Herein, the core–shell Co3O4@ZnIn2S4 S-scheme heterojunction was synthesized for achieving high-efficient photothermal-assisted photocatalytic hydrogen (H2) performance under full solar-spectrum irradiation. Notably, photocatalytic H2 production tests indicate that the as-prepared optimal Co3O4@ZnIn2S4 sample (CO@ZIS-20) exhibits impressive H2 production rates of about 18.9 and 9.8 mmol h−1 g−1 under AM 1.5G and real sunlight irradiation, respectively. The effect of the reaction solution temperature induced by the photothermal effect on the photocatalytic activity in solid–liquid reactions was also investigated. Furthermore, the results of the characterization analysis revealed that high-frequency photons dominate photocatalytic reactions while low-frequency photons are converted into heat to improve photocatalytic reactions. This study provides effective design ideas of developing high-activity photothermal-assisted photocatalysts for realizing solar energy conversion.

Full solar spectrum-driven Cu2O/PDINH heterostructure with enhanced photocatalytic antibacterial activity and mechanism insight

Marine biofouling hazards the sustainable development of the environment and has become a potential threat to environmental and ecological security. Photocatalytic antibacterial agents driven by the full solar spectrum are promising antifouling agents for environmental protection. The cuprous oxide/perylene-3,4,9,10-tetracarboximide (Cu2O/PDINH) heterostructure was successfully constructed by integrating p-type Cu2O and n-type PDINH to improve photocatalytic antibacterial efficiency. PDINH extended the absorption spectrum from ultraviolet to near-infrared, improving light utilization by 75 %. The Cu2O/PDINH heterostructure reduced the toxicity risk of Cu2O for environmental pollution, achieved full solar spectrum drive and overcame the inherent defect that Cu2O cannot produce singlet oxygen. The Cu2O/PDINH heterostructure exhibited excellent long-term and photocatalytic antibacterial activity with an antibacterial rate of > 90 % due to the sterilization of copper ions and the continuous generation of ROS driven by the full solar spectrum. This inorganic-organic Cu2O/PDINH heterostructure shows great application prospects in energy and the environment. The Cu2O/PDINH heterostructure with effective ROS increase and superior photocatalytic sterilization efficiency has great potential for environmentally friendly marine antifouling agents.

Z-scheme WOx/Cu-g-C3N4 heterojunction nanoarchitectonics with promoted charge separation and transfer towards efficient full solar-spectrum photocatalysis

Construction of Z-scheme heterojunctions has been considered one superb method in promoting solar-assisted charge carrier separation of carbon-based materials to achieve efficient utilization of solar energy in hydrogen production and CO2 reduction. One interesting concept in nanofabrication that has become trend recent years is nanoarchitectonics. A heterostructure photocatalyst constructed based on the idea of nanoarchitectonics using the combination of g-C3N4, metal and an additional semiconducting nanocomposite is investigated in this paper. Z-scheme tungsten oxide incorporated copper modified graphitic carbon nitride (WOx/Cu-g-C3N4) heterostructures are fabricated via immobilization of WOx on Cu nanoparticles modified superior thin g-C3N4 nanosheets. Mechano-chemical pre-reaction and a two-step high-temperature thermal polymerization process are the keys in attaining homogeneous distribution of Cu nanoparticles in g-C3N4 nanosheets. The horizontal growth of homogeneously distributed WOx nanobelts on Cu modified g-C3N4 (Cu-g-C3N4) base via solvothermal synthesis is achieved. The photocatalytic performances of the heterostructures are evaluated through water splitting and CO2 photoreduction measurements in full solar spectrum irradiation condition. The presence of Cu nanoparticles in the composite system improves charge transport between g-C3N4 and WOx and thus enhances the photocatalytic performances (H2 generation and CO2 photoreduction) of the composite material, while the presence of WOx nanocomposites enhances light absorption of the composite material in the near infrared range. The synthesized heterostructure with optimized WOx to Cu-g-C3N4 ratio and in case of no co-catalyst addition exhibits enhanced photocatalytic H2 evolution (4560 μmolg-1h−1) as well as excellent CO2 reduction rate (5.89 μmolg-1h−1 for CO generation).

A novel full solar light spectrum responsive antimicrobial agent of WS2 quantum dots for photocatalytic wound healing therapy.

Photocatalytic antimicrobial therapy (PCAT) is considered to be a potential therapeutic treatment for bacterial-infection diseases. However, the antibacterial efficiency is unsatisfactory due to the limited application scope of photocatalysis. In this work, full-spectrum responsive tungsten disulfide quantum dots (WS2 QDs) are prepared for killing bacteria and enabling wound healing through photocatalytic reactive oxygen species (ROS) generation and glutathione (GSH) depletion. On the one hand, these ultrasmall WS2 QDs exhibit an excellent full spectrum (UV-Vis-NIR)-responsive photocatalytic effect by hindering the recombination of electron-hole pairs, thereby achieving the full use of the energy spectrum. Furthermore, the full-spectrum photocatalytic property of the as-prepared WS2 QDs can be effectively strengthened by redox reaction to deplete GSH for accelerated wound healing. In a word, the as-prepared nanoplatform exhibits the ability to act as an admirable antibacterial reagent with full-spectrum catalytic performance for photocatalytic wound healing therapy. Therefore, this work will not only provide an effective full-spectrum photocatalytic reagent for anti-bacteria therapy and wound healing, but also provide a rational idea for the development of other novel antibacterial agents for applications in the biomedical field.

A ternary system exploiting the full solar spectrum to generate renewable hydrogen from a waste biomass feedstock

A solar-driven system is proposed capable of hydrogen production from waste biomass with low carbon and water footprints.

MODEL DEVELOPMENT AND PERFORMANCE IMPROVEMENT OF A PHOTOVOLTAIC-THERMOELECTRIC SYSTEM BY INTEGRATING AND OPTIMIZING PHASE CHANGE MATERIALS

Integrating phase change materials (PCMs) with concentrated photovoltaic-thermoelectric (PV-TE) systems can effectively control the interface temperature between PV and TE components and improve the full solar-spectrum utilization efficiency. However, since the structure of photovoltaic-phase change material-thermoelectric (PV-PCM-TE) systems is complex and the temperatures among the components are coupled and affect each other, the photo-thermal-electric conversion characteristics under the actual physical properties need to be analyzed by a more detailed model, and the suitable operating conditions for PV-PCM-TE systems remain clear. There is still a lack of the method for improving the system performance. Therefore, a three-dimensional transient model is established herein by combining the Monte Carlo ray-tracing method and finite volume method to simulate the complex energy conversion processes of the PV-PCM-TE system. Based on this, performances of PV-PCM-TE, PV-TE, and PV systems are compared under different operating conditions, and the applicable conditions for PV-PCM-TE systems are analyzed. Then effects of key parameters of the phase change module are investigated. In the end, to further improve the system performance, a partition screening method of PCM is proposed considering the nonuniform solar radiation on photovoltaic surfaces, and the selection and layout area of PCMs are optimized. The results present that the applicable operating conditions are low concentration ratio (< 20) and low heat transfer coefficient (< 20 W·m<sup>-2</sup>·K<sup>-1</sup>). In terms of structural parameters, the system power generation is most significantly affected by the width. In terms of PCM physical properties, it is most affected by the PCM density, followed by latent heat. For different concentration ratios, there are different optimal melting points to achieve the highest power generation. The proposed PCM partition screening method can efficaciously control PV-TE interface temperature, and reduce photovoltaic cells' temperature by 47°C. The system efficiency can be increased by 4.8% and 4.2% after the optimization compared with that of the single PV cell and the traditional PV-TE system, respectively.