Photocatalysis is considered as one of the promising routes to solve the energy and environmental crises by utilizing solar energy. Graphitic carbon nitride (g-C3N4) has attracted worldwide attention due to its visible-light activity, facile synthesis from low-cost materials, chemical stability, and unique layered structure. However, the pure g-C3N4 photocatalyst still suffers from its low separation efficiency of photogenerated charge carriers, which results in unsatisfactory photocatalytic activity. Recently, g-C3N4-based heterostructures have become research hotspots for their greatly enhanced charge carrier separation efficiency and photocatalytic performance. According to the different transfer mechanisms of photogenerated charge carriers between g-C3N4 and the coupled components, the g-C3N4-based heterostructured photocatalysts can be divided into the following categories: g-C3N4-based conventional type II heterojunction, g-C3N4-based Z-scheme heterojunction, g-C3N4-based p–n heterojunction, g-C3N4/metal heterostructure, and g-C3N4/carbon heterostructure. This review summarizes the recent significant progress on the design of g-C3N4-based heterostructured photocatalysts and their special separation/transfer mechanisms of photogenerated charge carriers. Moreover, their applications in environmental and energy fields, e.g., water splitting, carbon dioxide reduction, and degradation of pollutants, are also reviewed. Finally, some concluding remarks and perspectives on the challenges and opportunities for exploring advanced g-C3N4-based heterostructured photocatalysts are presented.

g-C3N4-Based Heterostructured Photocatalysts

Centralized water treatment has dominated in developed urban areas over the past century, although increasing challenges with this model demand a shift to a more decentralized approach wherein advanced oxidation processes (AOPs) can be appealing treatment options. Efforts to overcome the fundamental obstacles that have thus far limited the practical use of traditional AOPs, such as reducing their chemical and energy input demands, target the utilization of heterogeneous catalysts. Specifically, recent advances in nanotechnology have stimulated extensive research investigating engineered nanomaterial (ENM) applications to AOPs. In this Perspective, we critically evaluate previously studied ENM catalysts and the next-generation treatment technologies they seek to enable. Opportunities for improvement exist at the intersection of materials science and treatment process engineering, as future research should aim to enhance catalyst properties while considering the unique roadblocks to practical ENM implementation in water treatment.

Challenges and prospects of advanced oxidation water treatment processes using catalytic nanomaterials.

Herein, we proposed a new peroxymonosulfate (PMS) activation system employing the Fe(III) doped g-C3N4 (CNF) as catalyst. Quite different from traditional sulfate radical-based advanced oxidation processes (SR-AOPs), the PMS/CNF system was capable of selectively degrading phenolic compounds (e.g., p-chlorophenol, 4-CP) in a wide pH range (3–9) via nonradical pathway. The generated singlet oxygen (1O2) in the PMS/CNF3 (3.46 wt % Fe) system played negligible role in removing 4-CP, and high-valent iron-oxo species fixated in the nitrogen pots of g-C3N4 (≡FeV═O) was proposed as the dominant reactive species by using dimethyl sulfoxide as a probe compound. The mechanism was hypothesized that PMS was first bound to the Fe(III)-N moieties to generate ≡FeV═O, which effectively reacted with 4-CP via electron transfer. GC-MS analysis indicated that 4-chlorocatechol and 1,4-benzoquinone were the major intermediates, which could be further degraded to carboxylates. The kinetic results suggested that the formation of ...

Fe(III)-Doped g-C3N4 Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species.

Many organic and inorganic compounds have been developed as visible light driven photocatalysts for environment and energy application. In this work, a metal-free carbon doping–carbon nitride (BCM-C 3 N 4 ) nanocomposite was synthesized by introducing barbituric acid and cyanuric acid during the polymerization of melamine. The BCM-C 3 N 4 was characterized by structure, porosity, optical performance, and photoelectrochemical properties. Results demonstrated that BCM-C 3 N 4 sample exhibited higher surface area, lower fluorescence intensity, better photocurrent signals and more efficient charge transfer in comparison to pure C 3 N 4 . The BCM-C 3 N 4 exhibits excellent photocatalytic degradation ability of sulfamethazine (SMZ) under visible light irradiation. Much superior photocatalytic activity and high pollutant mineralization rate was achieved by BCM-C 3 N 4 , where it was 5 times than that of pristine C 3 N 4 . The effect of initial SMZ concentrations on photocatalyst was also investigated. Additionally, the trapping experiments and electron spin resonance tests demonstrated that the main active species, such as O 2 − and h + , could be produced under light irradiation. This work might provide an effective approach to the design of low-cost and highly efficient photocatalysis degradation systems for water treatment.

Highly porous carbon nitride by supramolecular preassembly of monomers for photocatalytic removal of sulfamethazine under visible light driven

g-C3N4界面改性:掺杂金属硫化物构建新型异质结光催化剂的能源转换展望

In Situ Stripline Electrochemical NMR for Batteries

The development of applications for germanium nanocrystals has been hindered by the limited availability of synthetic methods coupled with poorly understood ligand-exchange chemistry. Herein we describe the synthesis of germanium nanocrystals and ligand exchange experiments designed to establish facile routes toward ligand replacement and, consequently, layers that are amenable to charge-transfer. After assessing thiols, carboxylates, and dithiocarbamates, sulfur dissolved in 1-ocatadecene was determined to be the most amenable to ligand exchange, with over 95% of the initial alkylamine ligand replaced as determined by Fourier transform infrared spectroscopy (FTIR). These results were in good agreement with density functional theory calculations showing a strong preference for Ge–S bonding. The materials were fully characterized via powder X-ray diffraction, FTIR, transmission electron microscopy, and X-ray and UV photoelectron spectroscopy. This new ligand exchange procedure provides a possible route tow...

Sulfur-Capped Germanium Nanocrystals: Facile Inorganic Ligand Exchange

Novel Pd-based catalysts (i.e., Pd and Pd–Cu) supported on graphitic carbon nitride (g-C3N4) were prepared for nitrite and nitrate hydrogenation. The catalysts prepared by ethylene glycol reduction exhibited ultrafine Pd and Pd–Cu nanoparticles (∼2 nm), and they showed high reactivity, high selectivity toward nitrogen gas over byproduct ammonium, and excellent stability over multiple reaction cycles. The unique nitrogen-abundant surface, porous structure, and hydrophilic nature of g-C3N4 facilitates metal nanoparticle dispersion, mass transfer of reactants, and nitrogen coupling for nitrogen gas production to improve catalytic performance.

Graphitic Carbon Nitride Supported Ultrafine Pd and Pd–Cu Catalysts: Enhanced Reactivity, Selectivity, and Longevity for Nitrite and Nitrate Hydrogenation

We provide an efficient, sustainable, low-cost, and potentially scalable method to prepare N-functionalized activated carbon (AC) for Pd-based catalysis with improved performance for water purification. N-functionalized AC supports were realized via “soft nitriding”, that is, low temperature heating of a urea–AC mixture, and Pd nanoparticles with a significantly increased number of surface Pd(0) sites were achieved on the supports. Moreover, Pd nanoparticles were preferentially loaded near the (treated) AC exterior surface. N-functionalization improved nitrite and bromate hydrogenation kinetics but not for chlorite and chlorate, suggesting that different mechanisms determine the reaction activity of these oxyanions.

Pd Nanoparticle Catalysts Supported on Nitrogen-Functionalized Activated Carbon for Oxyanion Hydrogenation and Water Purification

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In Situ Stripline Electrochemical NMR for Batteries

Sulfur-Capped Germanium Nanocrystals: Facile Inorganic Ligand Exchange

Graphitic Carbon Nitride Supported Ultrafine Pd and Pd–Cu Catalysts: Enhanced Reactivity, Selectivity, and Longevity for Nitrite and Nitrate Hydrogenation

Pd Nanoparticle Catalysts Supported on Nitrogen-Functionalized Activated Carbon for Oxyanion Hydrogenation and Water Purification