Separation Efficiency Of Carriers Research Articles

Enhanced Charge Transfer in Poly(Heptazine Imide) Synergistically Induced by Donor‐Acceptor Motifs and Ohmic Junctions for Efficient Photocatalytic CO2 Reduction

Poly(heptazine imide) (PHI) has received widely interest in the photocatalytic CO2 reduction due to its good crystallinity and complete in‐plane structure. However, its poor photo‐induced carrier separation and migration efficiency and insufficient active sites results in undesirable photocatalytic CO2 reduction performance. Herein, we designed and constructed a novel ohmic junction photocatalyst by integrating melamine edge‐modified PHI (mel‐PHI) with extended π‐conjugated system with TiN (TiN/mel‐PHI) for enhancing the photocatalytic CO2 reduction activity. Strikingly, the photocayalytic CO2 reduction yield of the optimal TiN/mel‐PHI is 62.64 µmol·g–1·h–1, which is 5.6 and 2.8 times higher than PHI (11.26 µmol·g–1·h–1) and mel‐PHI (22.32 µmol·g–1·h–1), respectively. The superior photocatalytic CO2 reduction activity is attributed not only to the formation of D‐A structure by the introduction of melamine, which extends the π‐conjugation system, alters the electronic structure of PHI, and accelerates the charge separation and migration, but also to the induced internal electric field by ohmic junction further enhances the charge separation and migration efficiency. Meanwhile, the synergistic effect of mel‐PHI and TiN enriched the electron number of TiN, reducing the CO2 reduction potential. This work highlights the synergistic enhancement of charge transfer between D‐A motifs and ohmic junctions, confirming their potential in optimizing photocatalysts.

Cu/S Co-anchoring junction boosted the photogenerated carrier separation efficiency in g-C3N5 for enhanced H2 evolution

C3N5 is emerging as an important visible light catalyst because of its narrow band gap, nontoxicity and thermal stability. Herein, sulfur-doped g-C3N5 (SCN) was prepared by copolymerization of thioacetamide (TAA) and 3-amino-1,2,4-triazole (3-AT). Then copper nanoparticles (Cu NPs) were anchored onto the SCN framework, resulting in the formation of Cu/SCN. It was found that the average H2 production rate of SCN and Cu/SCN was 0.76 and 1.34 mmol g−1 h−1, which was much higher than that of C3N5, respectively. Acting as a new active spots, sulfur doping effectively reduces the band gap of g-C3N5, and the formation of S-Cu bonds further creates an efficient electron transport pathway. As a result, Cu/SCN possesses a broader visible light absorption spectrum, stronger reduction capability, and greater efficiency in photo-induced carrier separation and transfer. Therefore, this work introduces a novel strategy for design of high efficiency photocatalytic H2 evolution carbon nitride through non-noble metal and sulfur anchoring junction.

Reinforcing Photogenerated Carrier Extraction of Environment‐Friendly InP/ZnSeS Quantum Dots for High‐Performing Photoelectrochemical Photodetection and Solar Energy Conversion

AbstractColloidal InP/ZnSeS‐based quantum dots (QDs) are considered promising building blocks for light‐emitting devices due to their environmental friendliness, high quantum yield (QY), and narrow emission. However, the intrinsic type‐I band structure severely hinders potential photoelectrochemical (PEC) applications requiring efficient photoexcited carrier separation and transfer. In this study, the optoelectronic properties of InP/ZnSeS QDs are tailored by introducing Al dopants in the ZnSeS layer, which concurrently passivate the surface defects and act as shallow donor states for suppressed non‐radiative recombination and improved charge extraction efficiency. Consequently, as‐fabricated InP/ZnSeS:Al QDs‐based PEC‐type photodetector exhibited a high detectivity up to 1011 Jones and a remarkable responsivity of 0.66 A W−1 at 600 nm even under self‐powered condition (0V bias). In addition, as‐prepared InP/ZnSeS:Al QDs‐based photoanode can be alternatively used for PEC hydrogen generation, showing an H2 production rate of 73.7 µmol cm−2 h−1 under 1 sun illumination (AM 1.5G, 100 mW cm−2). The results offer a prospective strategy for optimizing eco‐friendly QDs for high‐performance multifunctional light detection/conversion devices.

Structural Design on Porous Aromatic Frameworks for Photocatalysis

Photocatalytic technology has shown great potential in various fields such as environmental purification, energy conversion, and chemical transformations due to its green, sustainable, and low‐cost characteristics. Porous aromatic frameworks (PAFs) with high specific surface areas, designable local structures, and abundant active sites could potentially serve as efficient photocatalysts for various catalytic reactions. This makes PAFs have a wide range of application prospects and significant advantages in the field of photocatalysis. This concept discusses the recent progress of photocatalysis over PAFs. Various strategies are used to solve the general problems of photocatalyst, such as poor light absorption, low carrier separation efficiency and poor stability, which further reveal the relationship between their structure and performance.

Fabrication and Mechanism Insight of Multidimensional Coupled Metal-Free van der Waals Heterostructures for Enhanced Photocatalytic Hydrogen Evolution.

It is an arduous issue to significantly improve the charge separation efficiency of polymer photocatalysts due to their inherently high exciton binding energy. Herein, based on an interfacial coupling and atom diffusion strategy, a metal-free 3D/2D van der Waals (VdW) heterojunction is fabricated through the modification of rich-vacancy wrinkle-like S8 (Vs-S8) microspheres on the surface of S-doped polymeric carbon nitride (S-PCN) nanosheets. The insight into the mechanism reveals that the interfacial coupling effect induces a strong built-in electric field from S-PCN to Vs-S8, and the carrier transfer behavior abides by the type-II charge transfer pathway, thereby dramatically improving the separation efficiency and transport kinetics of photogenerated carriers. As a result, the as-prepared metal-free 3D/2D Vs-S8/S-PCN VdW heterojunction is endowed with more superior photocatalytic hydrogen evolution (PHE) performance than PCN. The highest average PHE rate is about 11.3 times higher than that of PCN, and the apparent quantum efficiency reaches 30.1% at 400 nm on the optimal 3%-Vs-S8/S-PCN sample. This work contributes a new design strategy for a metal-free VdW heterojunction and provides a feasible avenue for improving the carrier separation efficiency of polymer photocatalysts.

Porphyrin-prompted robust lead-free cesium bismuth bromide for efficiently photodegrading antibiotics pollutants in water

The lead-free halide perovskite represented by Cs3Bi2Br9 (CBB) has attracted intense attention as an environmentally friendly alternative for toxic lead halide perovskite (CsPbBr3). However, the limited light absorption and instability of Cs3Bi2Br9 hinder its practical application in photocatalysis. In this work, Cs3Bi2Br9 nanosheets was modified with bifunctional porphyrin (CBB-TCPP) displayed enhanced visible light absorption properties and promising water stability. The CBB-0.5TCPP shows a sharply improved photodegradation performance of 84 % in 60 min in water and demonstrating the outstanding cycling stability. Furthermore, photoelectrochemical tests suggested that the charge separation and transfer properties of the modified perovskite materials were significantly improved compared with the pristine CBB. The CBB-0.5TCPP exhibited an impressive photogenerated carrier separation efficiency of 90.74 %. This work innovatively proposes a new way to modify perovskite with double duty by boosting stability and optimizing light absorption properties.

Advanced plasmonic few-layered InSe nanosheet heterojunctions for enhanced photoelectrochemical water splitting

The selenide-based Van der Waals heterojunctions show great potential for the next generation of photoelectronic nanodevices. Herein, we construct a 2D photoanode nanocatalyst that consists of ZnSe nanocrystals with exposed active surfaces coupled with few-layered InSe nanosheets decorated by Au nanoparticles. The resultant ZnSe/AuNPs@InSe multi-heterojunction photoanode demonstrates an outstanding photocurrent density of 4.86 mAcm−2 under AM 1.5 G simulated sunlight (100 mWcm−2), which is 8 times greater than that of the pristine InSe photoanode (0.61 mAcm−2). Moreover, the lifetime of photogenerated charge carriers is extended by a factor of 3. This significant enhancement in photoelectrochemical water splitting in the near-infrared region is attributed to the surface plasmonic effect produced by the modification of Au NPs when bulk InSe is exfoliated into multi-layered flakes. The interfacial coupling effects on carrier transfer dynamics, as revealed by impedance spectroscopy assisted with the First-Principal calculations, show that this photoanode significantly minimizes the internal resistance, boosts the charge carrier separation efficiency, and promotes water oxidation.

Ultra-thin FeVO4 modified Al-doped ZnO nanorods photoanode towards efficient photoelectrochemical water oxidation

Fabricating of high-performance photoanodes played an important role in achieving efficient conversion of solar energy to hydrogen energy. Herein, Al-ZnO/FeVO4 core–shell nanorods arrays (NRs) was constructed through a simple two-step method to form type-II heterojunction. Compared with the Al-ZnO substrate (0.55 mA/cm2), the modified Al-ZnO/FeVO4 photoanode exhibited superior photocurrent density, with an optimal photocurrent density of 1.13 mA/cm2 at 1.23 V vs. RHE (AM 1.5G). Heterogeneous structures suppressed the photoinduced bulk recombination of charge carriers and improved the separation efficiency of charge carriers. More importantly, the ultra-thin FeVO4 modification layer weakened surface capture states, increased photovoltage, and promoted interfacial charge transfer dynamics. This work provided new ideas for designing high-performance photoanodes.

Synthesis of CuOQDs/g-C3N4/C Composites Via Stem Template Induction and their Photocatalytic Properties

Introduction: The synthesis of bio-templated porous CuOQDs/g-C3N4/C composites with controllable morphology and suitable energy band structure was successfully carried out via a simple thermal condensation and hydrothermal method. Method: Dicyandiamide and cadmium chloride were selected as starting materials, while Hollyhock stem was chosen as the biological template. The results indicated that, in comparison to pure g-C3N4, g-C3N4/C had a rich porous structure and better-photogenerated carrier separation efficiency. The CuOQDs were anchored evenly on the surface of the g-C3N4, thus resulting in the formation of a greater number of reactive sites. Results: The type-Z heterojunction formed between the CuOQDs and g-C3N4/C reduced the energy required for electron transition, thereby facilitating the separation of photo-generated electronhole pairs. The highest photocatalytic degradation efficiency of CuOQDs/g-C3N4/C for tetracycline (TC) was 65.1%, which was 3.3 times that of pure g-C3N4. Conclusion: In the photocatalytic process, the main reactive species is O2−. The CuOQDs/g- C3N4/C synthesized by stem induction in multi-phase heterojunction form has a stable microstructure to improve the charge separation efficiency. Further, it represents practical photocatalytic environmental protection.

Degradation of carbamazepine in piezo-activation of persulfate systems: Comparison of PDS and PMS

The choice of persulfate (PS) is crucial to the degradation and energy efficiencies for piezo-activation of PS (PE-PS) systems. Herein, a comparison between piezoelectrically activated peroxydisulfate (PDS) and peroxomonosulfate (PMS) using BaTiO3 are comparatively investigated for carbamazepine (CBZ) degradation. By contrast, the PE-PMS system achieves better degradation and mineralization of CBZ, as well as higher reaction stoichiometric efficiencies (%RSE). Nevertheless, the energy consumption of the PE-PDS system is only 9.69% of the PE-PMS system. The quenching test, chemical probe determination, and electron spin resonance (EPR) analysis suggest that the concentration of •OH, SO4∙-, and 1O2 except ∙O2- of the PE-PMS system, is higher than that of the PE-PDS system. The piezoelectric current density and carrier separation efficiency of the PE-PMS system are higher than that of the PE-PDS system, demonstrating that the piezoelectrically activated PMS has higher reactivity than piezoelectrically activated PDS. The ∙O2- and •OH are the primary ROS in the PE-PDS system, while 1O2 and •OH are the major ROS in the PE-PMS system. Additionally, CBZ is effectively degraded by both PE-PMS and PE-PDS systems from actual water sources. This work compares the performance, energy cost, and mechanism of PE-PMS and PE-PDS systems systematically. Hopefully, all of that is designed to tender a helpful reference for the choice of PS in piezocatalytic research and application.

G-C3N4 coupled with GO accelerates carrier separation via high conductivity for photocatalytic MB degradation

Graphitic carbon nitride (g-C3N4) is widely utilized in photocatalysis due to its responsiveness to visible light, low cost, and non-toxicity. However, its efficiency is limited by factors such as the rapid recombination of photogenerated electron-hole pairs, slow electron transfer rates, and a limited number of active surface sites. In this study, g-C3N4 was synthesized through thermal polymerization, and varying amounts of graphene oxide (GO) were incorporated via physical blending to fabricate composite photocatalysts. The results indicated that the incorporation of GO not only increased the specific surface area and modified the pore size distribution of g-C3N4 but also affected the heptazine ring structure through chemical bonding, thereby enhancing the density of active sites. Photocatalytic degradation experiments with methylene blue (MB) indicated that g-C3N4 containing 2% GO exhibited photocatalytic activity 2.84 times greater than that of pristine g-C3N4. Kinetic simulations indicated that the Kapp value for the 2% GO-g-C3N4 composite was 0.00469min-1, which is 4.34 times higher than that of pure g-C3N4 (0.00108min-1). Furthermore, this composite maintained high photocatalytic activity after four cycles of reuse. An analysis of the photocatalytic degradation mechanism revealed that the incorporation of GO effectively promoted the separation and transfer of photogenerated electron-hole pairs, enhanced photocurrent density, and improved carrier separation efficiency. Electron spin resonance (ESR) and free radical scavenging experiments confirmed that the primary active species involved in the degradation of MB by the composite photocatalyst were ·O2- and h+. This study presents a novel approach for enhancing the photocatalytic performance of g-C3N4 by modifying its electronic structure and surface properties.

In situ construction of S-scheme heterojunctions between BiOCl and Bi-MOF for enhanced photocatalytic CO2 reduction and pollutant degradation

Recently, photocatalytic technology has been widely used as a sustainable method to address environmental pollution issues. Herein, BiOCl/Bi-MOF (BOC/Bi-MOF) based semiconductor photocatalysts with S-scheme heterojunction were fabricated by an in situ growth method, and the photocatalytic activity of the materials was explored for CO2 reduction and pollutant degradation. As confirmed by density functional theory calculations and physiochemical characterizations, the established S-scheme heterojunction confers enhanced carrier separation efficiency and retention of redox capability to the BOC/Bi-MOF. Through an improved combination of charge separation and surface reactions, the prepared BOC/Bi-MOF efficiently reduces CO2 solely to CO. The heterojunction as catalyst is more durable and effective than any of its single component. The CO evolution rate of the optimized composite catalyst was 7.66 and 33.10 times of those of BiOCl and Bi-MOF, respectively. In addition, BOC/Bi-MOF exhibits a high efficiency in the photocatalytic degradation of the pollutant rhodamine B (RhB) in aqueous environments, and the pollutant was completely removed within 20 min. Due to the generation of interfacial potential differences, the internal electric field (IEF) generation at heterogeneous interfaces facilitates the separation and transfer of photogenic charges. This work demonstrated a practical and effective route for in situ growth of S-scheme heterojunctions with high efficiencies in CO2 reduction and RhB degradation.

Modulation of the Microstructure and Enhancement of the Photocatalytic Performance of g-C3N4 by Thermal Exfoliation

This work explores the impact of reaction temperature during thermal exfoliation treatment of bulk-g-C3N4 in the air atmosphere on the structure and performance of the resulting CN photocatalyst. The analysis conducted using XRD, FT-IR, XPS, SEM, and elements mapping tests, illustrated an increase in nitrogen-vacancy and oxygen content on the surface of the CN photocatalyst, resulting in a porous and sparse structure, changes in crystal size, and improved visible light absorption performance. The photocatalytic reduction experiments of hexavalent chromium (Cr(VI)) showed that the CN-540 showed the highest reduction rate of 96.9%, with a reaction rate constant 6.21 times that of bulk-g-C3N4. After 100 min of illumination, the photocatalytic degradation rates of CN-540 for TC-HCl and RhB were 66.7% and 60.6%, respectively. The TOC test results indicated mineralization rates of 51.5% for TC-HCl and 46.6% for RhB. Room temperature fluorescence spectroscopy (PL), transient photocurrent response (TPC), and electrochemical impedance spectroscopy (EIS) measurements confirmed the excellent photogenerated charge carrier separation and transport efficiency of CN-540. The photocatalytic mechanism for reducing Cr(VI) by CN-540 was elucidated based on the active species •OH and •O2– and Mott-Schottky (M-S) tests. This study provides experimental data for optimizing the photocatalytic performance of g-C3N4 and paves a new way for developing efficient photocatalysts. Copyright © 2024 by Authors, Published by BCREC Publishing Group. This is an open access article under the CC BY-SA License (https://creativecommons.org/licenses/by-sa/4.0).

Tailoring Carrier Dynamics of BiVO4 Photoanode via Dual Incorporation of Au and Co(OH)x Cooperative Modification for Photoelectrochemical Water Splitting

AbstractPhotoelectrochemical solar to hydrogen production is a promising way to achieve carbon neutrality, but severe charge recombination in photoanodes limits the conversion efficiency. Herein, Au nanoparticles and Co(OH)x co‐sensitized bismuth vanadate (BiVO4) to construct AuCo(OH)x/BiVO4 photoanode for significantly enhancing the performance of photoelectrochemical water splitting. This process significantly improves the bulk charge carrier separation efficiency, the surface kinetics of water oxidation, and the electron density of BiVO4 photoanode through Au surface plasmon resonance (SPR) and Co(OH)x oxygen evolution catalysts effect. Additionally, the enhancement of the *O and the *OOH generation accelerate the oxygen evolution reaction kinetics. Consequently, the constructed AuCo(OH)x/BiVO4 photoanode demonstrates an excellent photocurrent of 6.2 mA cm−2 at 1.23 V versus reversible hydrogen electrode and a stable continuous output within 42 h. This work contributes to developing high‐efficiency and high‐stability photoanodes for solar H2 production through SPR effect and oxygen evolution catalysts.

Construction of direct Z-scheme Sn3O4/WO3 heterostructure photocatalyst for enhanced Congo red degradation and Cr(Ⅵ) reduction performance

The development of well-designed architectures is crucial in accelerating the transport of photon-generated carriers in composite photocatalysts. In this study, a direct Z-scheme Sn3O4/WO3 (SW) photocatalyst was successfully fabricated utilizing a straightforward hydro/solvothermal approach, where Sn3O4 nanosheets (NSs) grew in-situ onto WO3 nanorods (NRs) uniformly. The optimal SW-2 composite exhibits a remarkable reduction rate of 93.5 % for Congo Red (CR) within 40 min, with a rate constant (k) of 0.075 min−1. This performance surpasses that of pristine Sn3O4 and WO3, which have rate constants of 0.027 min−1 and 0.018 min−1, respectively. Additionally, the SW-2 composite effectively removes 89.2 % of Cr(VI) over 100 min, achieving a k value of 0.019 min−1, which is higher than that of Sn3O4 (0.013 min−1) and WO3 (0.001 min−1). Furthermore, the photocatalytic degradation performance of the recovered samples retains their photocatalytic degradation performance after five consecutive experimental cycles, indicating excellent durability. The enhanced photocatalytic performance can be attributed to the construction of a direct Z-scheme heterostructure, which not only broadens the spectral response range, bur also ensures efficient separation of photoexcited carriers and fosters robust photo-redox capacity within the composite. This study is expected to provide some valuable insights into the design and synthesis of Z-scheme heterojunction photocatalysts, aimed at addressing pressing environmental pollution challenges.

Boosting Photoelectrochemical Water Oxidation Performance of Ti–Fe2O3 Photoanode via NH2–MIL–53(FeCo) as a Cocatalyst

α–Fe2O3 is a promising photoanode that can be used for solar‐driven photoelectrochemical (PEC) water splitting. However, due to low carrier separation efficiency and slow water oxidation kinetics, the PEC performance of Ti–Fe2O3 is still severely hindered. Here, a novel inorganic–organic hybrid composite photoanode is prepared by depositing NH2–materials of institute Lavoisier (MIL)–53(FeCo) cocatalyst on the surface of Ti–Fe2O3 using solvothermal method. In the results, it is shown that the Ti–Fe2O3/NH2–MIL–53(FeCo) photoanode has a high photocurrent density (3.0 mA cm−2 at 1.23 V vs reversible hydrogen electrode (RHE), which is 5.1 times that of bare Ti–Fe2O3, and the initial potential of water oxidation also undergoes a negative change of about 100 mV. The separation efficiency of Ti–Fe2O3/NH2–MIL–53(FeCo) is significantly enhanced, and the charge injection efficiency increases from 17.6% to 68% at 1.23 V versus RHE. In the further research, it is suggested that the excellent PEC performance of Ti–Fe2O3/NH2–MIL–53(FeCo) may be attributed to an increase in carrier density, prolonged carrier recombination time, and an increase in exposed reactive sites. In this study, a new understanding for the design of Ti–Fe2O3 photoanodes with superior PEC performance based on metal organic framework modification is provided.

Bias‐Induced Gradient Bandgap of Bulk Perovskite Boosting Built‐In Electric Fields for High‐Performance Self‐Powered Photodetectors

AbstractSelf‐powered photodetectors (PDs) have gained significant attention in recent years due to their ability to operate without external power. Strengthening the built‐in electric field (Ebi) of these devices is crucial for efficient carrier separation and transport. However, the disordered energy level arrangement within mixed halide perovskites (MHP) often conflicts with the energy levels constructed by the external interface, weakening the Ebi and thus affecting the performance of self‐powered PDs. In this study, a bias‐induced gradient bandgap of bulk MHP is proposed for high‐performance self‐powered photodetectors. The vector superposition of the bias‐induced gradient bandgap with the interface electric field significantly boosts the Ebi of the device, providing a powerful driving force for the separation and transport of photogenerated carriers. The obtained device exhibits exceptional performance, including an ultra‐fast response time of 1.14/1.75 µs, a large specific detectivity of 7.27 × 1012 cm Hz1/2 W−1, an ultra‐high responsivity of 0.49 A W−1, and an external quantum efficiency of 93.5% at 0 V bias. Furthermore, this strategy is also demonstrated in lateral structure photodetector. This work offers valuable guidance for achieving high‐performance MHP‐based self‐powered PDs through bias‐induced gradient bandgap optimization.

Heterogeneous visible-light photoredox catalysis with NiCl2@g-C3N4 for induced C(sp2)-H/N[sbnd]H cross-dehydrogenative coupling

A novel photoactive NiCl2@g-C3N4 catalyst system, which effectively drives C(sp2)-H/NH bond formation between quinolin-2(1H)-ones, primary and secondary aliphatic amines under blue light irradiation. The NiCl2@g-C3N4 composite with a NiCl2 loading of 0.7wt% had the highest photoactivity, and the calculated band gap energy value is 2.56 eV The nickel ion could act as an electron acceptor enhancing carrier separation and transfer efficiency, greatly enhanced the photoreaction efficiency of g-C3N4. Preliminary mechanistic studies indicate upon visible light irradiation, the photo-generated electrons and holes act as oxidants, thereby generating amine radicals in the absence of external chemical oxidants. This provides a straightforward and efficient approach for directly 3-aminating quinoxalines-2(1H)-ones. Moreover, the heterogeneous catalyst can be recycled at least six times without significant activity loss.

Photoinduced Zn-Air Battery-Assisted Self-Powered Sensor Utilizing Cobalt and Sulfur Co-Doped Carbon Nitride for Portable Detection Device.

Most self-powered electrochemical sensors (SPESs) are limited by low open circuit voltage and power density, leading to a narrow detection range and low sensitivity. Herein, a photoinduced Zn-air battery-assisted SPES (ZAB-SPES) is proposed based on cobalt and sulfur co-doped carbon nitride with the cyano group (Co, S-CN). The cyano functionalization remarkably enhances visible light utilization, and the cyano moiety acts as an electron-withdrawing group to promote electron enrichment. Co and S co-doping can create a p-n homojunction within carbon nitride, enabling the efficient migration and separation of carriers, thereby significantly improving the performance of the oxygen reduction reaction. The synergistic effects endow Co, S-CN photocathode with an open circuit voltage of 1.85V and the maximum power density of 43.5µW cm-2 in the photoinduced ZAB. Employing heavy metal copper ions as the target model, the photoinduced ZAB-SPES exhibited dual-mode and sensitive detection. Furthermore, a portable detection device based on the photoinduced ZAB-SPES is designed and exhibits high linearity in the range of 5 ~ 600nM with a detection limit of 1.7nM. This work offers a portable detection method based on the photoinduced ZAB-SPES in the aquatic environment.

Vapor-Solid Interface Synthesis of Highly Crystalline Covalent Triazine Frameworks for Use as Efficient Photocatalysts.

Harsh synthetic conditions for crystalline covalent triazine frameworks (CTFs) and associated limitations on structural diversities impede not only further development of functional CTFs, but also practical large-scale synthesis. Herein, a mild and universal vapor-solid interface synthesis strategy is developed for highly crystalline CTFs employing trifluoromethanesulfonic acid vapor as catalysts. A series of highly ordered simple and functional CTFs (CTF-TJUs) can be facilely produced. In particular, the porphyrin-involved functional CTF (CTF-TJU-Por1) with high crystallinity is synthesized for the first time via this universal approach. The mechanism of vapor-catalyzed trimerization of nitrile monomers is thoroughly investigated through semi in situ characterizations. As a proof of concept, the photocatalytic performance of synthesized CTFs for water splitting is evaluated. CTF-TJU-133 exhibits significantly greater photocatalytic rates for hydrogen (4.35µmolh-1) and oxygen (2.18µmolh-1) evolutions during overall water splitting under visible light irradiations compared to other CTF-TJUs, representing one of the highest values among reported CTF photocatalysts. Further studies reveal that enhanced photocatalytic performance of CTF-TJU-133 results from optimized band structure, extended visible-light absorption, and high carrier separation efficiency. This study provides a promising strategy to synthesize various simple and functional CTFs, which significantly enriched diversities of CTF family for different application purposes.