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A palladium supported on graphitic carbon nitride (Pd/g-C3 N4 ) catalyzed carbonylative reaction of aryl bromides and arylboronic acids by has been developed for the construction of diaryl ketones. Using benzene-1,3,5-triyl triformate (TFBen) as the CO source, the reaction proceeded well to give various diaryl ketones in moderate to good yields.

Metal phthalocyanine has been extensively studied as a catalyst for degradation of carbamazepine (CBZ). However, metal phthalocyanine tends to undergo their own dimerization or polymerization, thereby reducing their activity points and affecting their catalytic properties. In this study, a catalytic system consisting of O-bridged iron perfluorophthalocyanine dimers (FePcF16-O-FePcF16), multi-walled carbon nanotubes (MWCNTs) and H2O2 was proposed. The results showed MWCNTs loaded with FePcF16-O-FePcF16 can achieve excellent degradation of CBZ with smaller dosages of FePcF16-O-FePcF16 and H2O2, and milder reaction temperatures. In addition, the results of experiments revealed the reaction mechanism of non-hydroxyl radicals. The highly oxidized high-valent iron-oxo (Fe(IV)=O) species was the main reactive species in the FePcF16-O-FePcF16/MWCNTs/H2O2 system. It is noteworthy that MWCNTs can improve the dispersion of FePcF16-O-FePcF16, contributing to the production of highly oxidized Fe(IV)=O. Then, the pathway of CBZ oxidative degradation was speculated, and the study results also provide new ideas for metal phthalocyanine-loaded carbon materials to degrade emerging pollutants.

Photocatalytic conversion of CO2 into value-added chemicals is considered to be a promising strategy to capture greenhouse gas as well as produce energy. The exploration of efficient and stable photocatalysts is crucial to promote CO2 reduction. Herein, we report the synthesis of a heterogeneous catalyst by integration of iron phthalocyanine (FePc) with g-C3N4via a simple reflux method, in which FePc works as the catalytic center and g-C3N4 acts as the photosensitizer. After 12 h of light irradiation, the CO yield by using the FePc/g-C3N4 catalyst is found to be 1696.96 μmol g−1 and no liquid products are detected. The mechanism for CO2 photoreduction over the FePc/g-C3N4 hybrid catalyst is proposed. To enhance its practicality and portability, we further load the powder catalyst on polyester fibers (PET). The obtained FePc/g-C3N4@PET exhibits high activity for CO2 reduction under both simulated and natural sunlight, with a CO yield of 493.35 μmol g−1 and 490.53 μmol g−1, respectively in 12 h. This work may pave the way to develop an approach for fabricating high-efficient 2D artificial photosynthetic systems for CO2 reduction.

Realizing high energy-density and actual applications of fibre-based electrochemical supercapacitors (FESCs) are pivotal but challenging, as the ability to construct advanced fibres for accelerating charges kinetic diffusion and Faradaic storage remain key bottlenecks. Here, we demonstrate high-performance FESCs based on hetero-structured polymetallic oxides/porous graphene core-sheath fibres, where the large pseudo-active polymetallic oxide (PMO) sheath is uniformly loaded on a hierarchical porous graphene fibre (PGF) core. Due to the abundant micro-/mesoporous pathways, large accessible surface, excellent redox activity and good interface electron conduction, the PMO-PGF possesses high areal capacitance (2959.78 mF cm

Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis. However, the traditional problems such as high recombination rate of photogenerated carriers limit its application. In this work, we introduce nitrogen deficiency into g-C

As some of the most promising alternatives to traditional non-degradable materials, photodegradable materials have advantages of environmental benignity and rapid degradation under simple conditions. In this work, nontoxic TiO

It is of great significance for improving electron transmission performance by changing of the outer ring structure of iron phthalocyanine. Herein, 4 (pyridine-2, 3-yl) iron phthalocyanine (FepyPc), as N-rich pyridyl-iron phthalocyanine derivative, was introduced to degrade pharmaceutical contaminants. The catalytic degradation of organic pollutants with FepyPc was studied by activating peroxymonosulfate (PMS) at room temperature. The results clarified that the removal rate of carbamazepine (CBZ) was close to 100% within 60 min and the calculated apparent rate constant was about 2 times larger than FePc, which proved that FepyPc had superior performance. Four active species were identified for the degradation of CBZ, including superoxide radical (•O

Iron-based metal-organic frameworks (Fe-MOFs) have been considered competitive catalyst candidates for the effective degradation of organic pollutants via advanced oxidation processes (AOPs) due to their unique porous architecture and tunable active site structure. However, little is known about the role of synergetic relationship between porous architecture and active site exposure of Fe-MOFs on catalysis for AOPs yet. Here, we demonstrated an overlooked compromise over these two features on modulating the catalytic ozonation reactivity of MIL-53(Fe) through a timescale-dependent crystal evolution. Enabled by intramolecular hydrogen bonds, the MIL-53(Fe) was subjected to six evolution steps in terms of crystal morphology, leading to a volcano plot of catalytic ozonation reactivity for Rhodamine B (RhB) degradation versus the crystallization time. Evidence suggested that the surface area of MIL-53(Fe) decreased dramatically, while the density of accessible active site increased when prolonging crystallization time, allowing for the facile modulation of catalytic ozonation reactivity of MIL-53(Fe). Electron paramagnetic resonance and fluorescence quantification tests verified that the screened MIL-53(Fe)s had a much better capacity for ∙OH generation than benchmark ozonation catalyst α-MnO

Palladium nanoparticles supported on low-melting polyester (Pd/LMPET) fabric were prepared through a microwave irradiation assisted method. In this way, in situ growth of Pd nanoparticles onto an easy to handle material was initiated and proceeded. The results of the characterization revealed that the palladium nanoparticles were well-dispersed on the surfaces of the polyester fibers. The Pd/LMPET fabrics were then employed in the Suzuki-Miyaura coupling. They exhibited excellent catalytic activity in ethanol/water under air atmosphere at 50 °C. Importantly, the Pd/LMPET fabrics could be separated from reaction mixture conveniently and they can still maintain good activity after 8 cycles without Pd leaching. © 2021 The Authors

Abstract Generally, the sulfate (SO4·−) and hydroxyl (HO·) radicals are the dominant active species in most catalytic oxidation processes with peroxymonosulfate (PMS). However, the existence of various natural organic and inorganic matters in aquatic environments might influence the oxidation efficiency of these radicals, and/or form more toxic and refractory intermediates than the parent, especially in chlorine-ion-containing conditions. Here, we constructed a novel visible-light catalytic system with PMS based on iron hexadecachlorophthalocyanine-poly (4-vinylpyridine)/polyacrylonitrile nanofibers through pyridine ligands to generate high-valent iron-oxo (Fe(IV)=O) species as the main active species. The coordination structure was characterized by UV–Vis diffuse reflection, X-ray photoelectron spectroscopy, etc. The high-valent iron-oxo generation from peroxysulfate O–O bond heterolytic cleavage was proved by high-definition electrospray ionization mass spectrometer. Ultra-performance liquid chromatography coupled with high-definition mass spectrometry showed that the photocatalytic system was efficient for the degradation of carbamazepine and the chlorinated intermediates by iron-oxo active species in chlorine-ion-containing conditions. Graphic Abstract

Solar-driven conversion of arylboronic acids to phenols was achieved by employing graphitic carbon nitride (g-C3N4) as heterogeneous photocatalyst, where O2− was the main active species. By loading g-C3N4 onto the easy weaving low melting point sheath-core composite polyester fibers (LMPET), g-C3N4-based artificial photosynthetic catalytic fabric (g-C3N4/LMPET) with a large light receiving area was prepared. It displayed the efficient conversion of arylboronic acid and excellent recycling performance. This system offers more possibilities to construct an artificial photosynthetic system with excellent solar-to-chemicals conversion efficiency.

The comfortable, beautiful and healthy residential environment has been a target pursued by human beings. However, the inevitable presences of indoor air pollutants such as nicotine which release from tobacco smoking imperceptibly invade people's health. Here, we developed new pigments consisted by colorful graphitic carbon nitride (g-C3N4)-based catalysts, which were fabricated by facile calcining and water bath refluxing procedures. The catalytic pigments exhibited a high catalytic activity for the removal of nicotine under sunlight or even light emitting diode (LED). The designed experiments revealed that superoxide radicals ( O2−) were main active species in g-C3N4-based catalysts system and played a significant role in removing contaminants. Noteworthy, the catalysts as pigments were successfully used for coloring textiles and painting. Both the catalytic textiles and paintings were provided with preferably photocatalytic performance and reusability. The catalytic pigments were simple to prepare, brightly colored and could effectively degrade nicotine, thus not only have decorative effect, enriching the spiritual world, but also contribute to the protection of the environment of human life.

Broad solar light absorption and rapid photogenerated electron-hole pair separation are two critical factors for the efficient enhancement of catalytic performance in a g-C3N4-based photocatalytic system. This study developed a facile method to construct a ternary graphitic carbon nitride/zinc tetracarboxyphthalocyanine/graphene quantum dots (g-C3N4/ZnTcPc/GQDs) composite photocatalyst. Graphene quantum dots (GQDs) were used to modify g-C3N4/ZnTcPc through hydrothermal method, where g-C3N4/ZnTcPc was fabricated by immobilizing zinc tetracarboxyphthalocyanine (ZnTcPc) onto g-C3N4 covalently via amido bonds. The photocatalyst was characterized by transmission electron microscopy, ultraviolet-visible diffuse reflectance spectrum, and X-ray photoelectron spectroscopy. The g-C3N4/ZnTcPc/0.1GQDs composites presented an increased photocatalytic activity by using Rhodamine B, sulfaquinoxaline sodium and carbamazepine as the model pollutants under solar light irradiation. ZnTcPc bonding on the g-C3N4 broadens its visible-light spectral response, and GQDs promotes the photogenerated electron-hole-pair separation efficiency because of its efficient electrons-transfer property. Experiments confirmed that superoxide radicals, photogenerated holes and singlet oxygen are the primary active species. The photocatalytic degradation pathway of Rhodamine B, sulfaquinoxaline sodium and carbamazepine was proposed on the basis of ultra-performance liquid chromatography and high-definition mass spectrometry.

Flexible and portable supercapacitors have been intensively investigated due to their reliable energy storage performance and promising applications in wearable electronic devices. Owing to the unique pseudocapacitance property of conducting polymer and the high conductivity and stability of carbon nanotube film (CNTF), polypyrrole (PPy) was electrodeposited on He plasma etched carbon nanotube film (HCNTF) for electrodes of flexible supercapacitor with high performance. As demonstrated by Raman spectra and contact angle measurement, He plasma etching can produce amorphous carbon on the CNTF and advance the hydrophilicity of the CNTF, which promoted the electrodeposition of PPy onto the CNTFs and improved the adhesion between PPy and CNTF. All-solid-state supercapacitors were fabricated using the PPy/HCNTF electrodes and H3PO4/PVA electrolyte. Cyclic voltammetry tests showed that the capacitive performance of PPy/HCNTF is much higher than that of PPy/CNTF. The specific capacitance of the PPy/HCNTF supercapacitor determined by a galvanostatic charge-discharge method at 0.5 A g−1 is about 414 F g−1, which was maintained 92% after 5000 cycles, reflecting high cycle stability. Moreover, the PPy/HCNTF supercapacitor could remain 96% of the original capacitance when it was bent for 500 times surrounding a cylinder with a diameter of 1.5 cm, showing perfect flexibility and great potential for flexible energy storage devices.

Current environmental concerns have encouraged researchers to search for a facile, environmentally-friendly and efficient method for sewage treatment. Cellulose aerogels (CAs) with high porosities, large specific surfaces and sustainability are promising candidates as catalytic carriers to solve many environment problems. However, pure CAs often lack mechanical strength and are prone to collapse under a small force, especially in water. Here, blended polyester fibers (B-PET) were used to support a CA containing nanosheet graphitic carbon nitride (g-C3N4), which greatly enhanced the tensile strength of the pure CA. Moreover, the composited aerogel, g-C3N4@CA/B-PET, showed high impact resistance in the water impact experiment and maintained its robust structure after 24 h of water shock. The g-C3N4@CA/B-PET exhibited a favorable photocatalytic activity towards the removal of hexavalent chromium and antibiotics simultaneously, which could challenge freestanding g-C3N4. The as-prepared composite material could be reused easily and maintained its excellent photocatalytic performance in cycling tests. Finally, the possible pathway for the degradation of sulfaquinoxaline and the mechanism in this photocatalytic system were proposed, where the superoxide radicals ( O2−) were the dominant active species, resulting in the oxidation of antibiotics. In addition, the photoelectrons could reduce the toxic hexavalent chromium to harmless trivalent chromium.

Utilizing peroxymonosulfate (PMS)-based advanced oxidation processes to remove emerging contaminants in water has received widespread attention. In this study, g-C3N4-IMA-FePcCl16 that was fabricated by axial coordination was applied to activate PMS for carbamazepine (CBZ) degradation. The introduction of imidazole-based ligand (IMA) and iron hexadecachlorophthalocyanine (FePcCl16) facilitates the photogenerated electron-hole pairs separation of g-C3N4 and broadens the visible-light response range. The coordination structure was characterized by X-ray diffraction and X-ray photoelectron spectroscopy. Photocatalytic experiments demonstrated that g-C3N4-IMA-FePcCl16 can highly effective eliminate CBZ with a removal of ∼95% within 25 min in the presence of PMS. The effects of various experimental parameters on the CBZ degradation were investigated, such as the loading amount of FePcCl16, pH, PMS dosage and anions. It is noteworthy that Cl− has a positive effect on the degradation of CBZ. Another interesting finding is that the degradation of CBZ is attributed to the synergistic effect of multiple active species, which is confirmed by gas chromatography-mass spectrometry, electron paramagnetic resonance and radical quenching tests. Superoxide radicals (O2 −) and singlet oxygen (1O2) are the dominated active species. This work offers a novel idea for the rational design of high-efficiency photocatalysts for wastewater remediation.

The current environmental problems urgently require researchers to seek an environmentally friendly, effective and easy to operate sewage treatment method. Graphite carbon nitride (g-C3N4), which has the advantages of simple preparation, safety, non-toxicity and chemical resistance, was expected to become a photocatalyst for solving environmental pollution. However, the performances of g-C3N4 still have some limitations that the electron hole recombination is fast and the powder is not easy to recover. In this study, zinc-doped graphite carbon nitride photocatalyst (Zn-g-C3N4) was mixed with polyacrylonitrile (PAN) to produce photocatalyst fibers by electrospinning. It not only solves the problem that the powder catalyst is difficult to recycle, but also effectively inhibits the recombination of photoelectron-hole pairs. Zn-g-C3N4/PAN has good photocatalytic activity for the simultaneous reduction of hexavalent chromium and degradation of pharmaceuticals. When organic pollutants are present, the reduction efficiency of hexavalent chromium was improved without affecting its own removal efficiency. The potential application value of Zn-g-C3N4/PAN catalytic fiber was further explored by simulating the complex actual water environment. The composite fiber can be easily reused and keep its superior photocatalytic performance. The mechanism of pharmaceuticals degradation was proposed, in which •O2 – is the most important active species, which leads to the oxidation of pharmaceuticals. Besides, the photoelectrons generated by the catalyst can reduce the toxic hexavalent chromium.The efficiency of Zn-g-C3N4 to remove pollutants is improved by PAN fiber as a carrier, which not only solves the problem of difficult recovery of powder catalysts, but also provides more active sites.

Developing efficient and environmentally friendly catalytic system is significant for the removal of sulfide in fuel. O-bridged diiron perfluorophthalocyanine/4-mercaptopyridine (FePcF16-O-FePcF16/4-Mpy) as a novel composite catalyst was designed and prepared by axial coordination. The catalyst characterization was conducted through ultraviolet-visible spectroscopy, fourier transform infrared spectroscopy, X-ray diffractometry, electrospray ionization–mass spectrometry and density-functional theory technology. A high-efficient extraction oxidative desulfurization system is composed of hydrogen peroxide (H2O2), the mixture of ethanol and water and FePcF16-O-FePcF16/4-Mpy. Notably, the coordination of 4-Mpy greatly enhanced the catalytic activity of FePcF16-O-FePcF16, 99.4% of the desulfurization rate was achieved in 20 min at 30 °C. The catalyst system was cycled 8 times without significantly reducing the removal of dibenzothiophene. Electron paramagnetic resonance and gas chromatography–mass spectroscopy proved the high-valent iron-oxo intermediates were the main active substances in the FePcF16-O-FePcF16/4-Mpy/H2O2 system, and the pathway of catalytic oxidation DBT was proposed. This work provided useful insights to select suitable ligands to improve the activity of metal phthalocyanine, and offered a novel idea for the construction of efficient oxidative desulfurization system.

A new procedure on palladium-catalyzed carbonylative cyclization of N-(2-pyridyl)sulfonyl (N-SO2Py)-2-iodoanilines with terminal alkenes has been developed for the expedite construction of dihydroquinolin-4(1H)-one scaffolds. Enabled by the chelating group and using benzene-1,3,5-triyl triformate (TFBen) as the CO source, both aromatic and aliphatic alkenes were smoothly transformed into the corresponding 2,3-dihydroquinolin-4(1H)-ones in good yields with excellent regioselectivities. Notably, the reaction of aromatic alkenes produces 2-aryl-2,3-dihydroquinolin-4(1H)-ones, while 3-alkyl-2,3-dihydroquinolin-4(1H)-ones were obtained when aliphatic alkenes were used. This protocol has been applied in the synthesis of antitumor agent A as well.

The overuse of antimicrobials has resulted in serious damage to the ecosystem and human health. Therefore, the development of an efficient, stable, and reusable catalyst to eliminate antimicrobials under mild conditions is highly desired. Drawing inspiration from the metabolism of drugs by the enzymes in the human body, such as heme catalase, we developed a simulated enzyme catalyst, perchloride iron phthalocyanine (FePcCl