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The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO 2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO 2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5 d and S 2 p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO 2 reduction. As a result, the product generation rate of Au SA /Cd 1−x S manifests a remarkable at least 113-fold enhancement compared with pristine Cd 1−x S. The electron density of reactive sites significantly affects catalytic performances. Here, authors demonstrate the electron density of different reactive sites can be modulated by regulating the type of vacancy and the size of Au, leading to effective CO 2 photoreduction.

Photocatalytic production of green oxidation reagents as an economical and environmental-friendly process is a promising strategy to replace the traditional production processes. In the present study, a series of 1.0 wt% Pt/WO3 photocatalysts with different surface chemical states of Pt were successfully fabricated. The different surface metallic Pt (Pt0) and oxidized Pt (PtOx) ratios on WO3 showed significant effects on the photocatalytic activities for strong oxidants of peroxydisulfate (S2O82-) and hydrogen peroxide (H2O2) formations. It is proposed that surface Pt0 and PtOx functioned as reduction site for O2 reduction to H2O and oxidation site for H2O oxidation to H2O2, respectively, during the photocatalytic process. As a result, a higher surface composition of Pt0 prepared using photodeposition (PD) method led to the formation of higher amount of S2O82-. On the other hand, PtOx-loaded WO3 using impregnation (IM) method showed significant formations of S2O82- and H2O2 simultaneously. This work provided a new idea for the design of noble metal Pt-supported WO3 for efficiently photocatalytic generation of S2O82- and H2O2.

Methane photooxidation into methanol offers a practical approach for the generation of high‐value chemicals and the efficient storage of solar energy. However, the propensity for C─H bonds in the desired products to cleave more easily than those in methane molecules results in a continuous dehydrogenation process, inevitably leading to methanol peroxidation. Consequently, inhibiting methanol peroxidation is perceived as one of the most formidable challenges in the field of direct conversion of methane to methanol. This review offers a thorough overview of the typical mechanisms involved radical mechanism and active site mechanism and the regulatory methods employed to inhibit product peroxidation in methane photooxidation. Additionally, several perspectives on the future research direction of this crucial field are proposed. This review presents a comprehensive summary of the typical mechanisms employed to inhibit methanol peroxidation, including both the radical mechanism and the active site mechanism, and related various methods for modifying photocatalysts to effectively suppress methanol peroxidation during the methane photooxidation process are summarized. Additionally, several perspectives on the future research direction of this crucial field are proposed.

BiOCl has been used in the photoreduction of CO 2 , but exhibits limited photocatalytic activity. In this study, Bi was in situ reduced and deposited on the surface of (001)-dominated BiOCl nanosheets by NaBH 4 to form Bi/BiOCl nanosheets enriched with oxygen vacancies. The as-prepared Bi/BiOCl nanosheets having low thickness (ca. 10 nm) showed much higher concentration of oxygen vacancies compared to Bi/BiOCl nanoplates having high thickness (ca. 100 nm). Subsequently, the photocatalytic activity of the Bi/BiOCl nanosheets enriched with oxygen vacancies for CO 2 reduction was dramatically enhanced and much higher than that of BiOCl nanoplates, nanosheets, and Bi/BiOCl nanoplates. It showed that the improved photocatalytic activity in the reduction of CO 2 can be attributed to the enhanced separation efficiency of photogenerated electron–hole pairs of the oxygen vacancies on BiOCl nanosheets and Bi metals. This work demonstrated that the in situ reduction of non-noble metals on the surface of BiOCl nanosheets that are enriched with oxygen vacancies is favorable for increasing photocatalytic CO 2 reduction.

Methane dry reforming not only utilizes two potent greenhouse gases of methane and carbon dioxide, but also provides a valuable feedstock for the production of chemicals. However, this process has been heavily hindered by high operating temperature and coke formation with catalyst deactivation over the last century. Herein, we propose an approach whereby concentrated-solar catalytic methane dry reforming addresses these longstanding issues. By leveraging focused light as the sole energy source and utilizing a well-designed catalyst, the catalyst with Ni-O 4 coordination active center achieves high conversion rates of 93.6% for CH 4 and 93.7% for CO 2 , meanwhile sustaining stability for over 800 hours. Particularly noteworthy is the light-to-chemical energy conversion efficiency reaching 25.9%. This research represents a significant leap forward in integrating renewable energy sources with chemical production, offering a viable and sustainable alternative to traditional thermochemical processes for generating valuable chemicals. Dry reforming of methane (DRM) supports the circular economy and energy sustainability, yet its application is limited by high operating temperatures and coke formation. Here, the authors introduce a concentrated-solar catalytic DRM strategy that overcomes these challenges.

The escalating demand for sophisticated carbon products, including carbon black, carbon nanotubes (CNTs), and graphene, has yet to be adequately addressed by conventional techniques with respect to large‐scale, efficient, and controllable carbon material synthesis. Molten pyrolysis emerges as a propitious strategy for generating such high‐value carbon materials. Abundant carbon sources encompassing methane (CH 4 ), carbon dioxide (CO 2 ), biomass, and plastics can undergo thermal decomposition into carbon constituents within molten metal or salt media. This methodology not only obviates dependence on traditional fossil fuels but additionally enables modulation of carbon material morphologies by varying the molten media, thereby presenting substantial potential for effective and controlled carbon material fabrication. In this review, we examine the capacity of molten pyrolysis in producing high‐value carbon materials derived from CH 4 , CO 2 , biomass, and plastics. Concurrently, we present a detailed overview of the potential applications of this novel methodology, particularly emphasizing its relevance in the fields of supercapacitors, flexible materials, and electrochemical cells. Furthermore, we contemplate future trajectories for molten pyrolysis, accentuating that amalgamation with auxiliary processes or technologies—like renewable energy systems and carbon capture and storage—represents a remarkably promising route for continued investigation.

Pyrolysis of methane is a carbon-economic method to obtain valuable carbon materials and CO x -free H 2 , under the carbon peaking and carbon neutrality goals. In this work, we propose a methane pyrolysis process to produce graphite and H 2 using bubble column reactor containing NiO/Al 2 O 3 and NaCl–KCl (molten salt). The process was optimized by the different amounts of NaCl–KCl, the CH 4 /Ar ratio and temperature, indicating that the CH 4 conversation rate could reach 92% at 900 °C. Meanwhile, we found that the addition of molten salt could obtain pure carbon materials, even if the conversation rate of CH 4 decreases. The analysis of the carbon products revealed that graphite could be obtained.

The exploration of visible light-responsive, efficient, and durable photocatalysts is of great concern for removing organic dyes and antibiotics from wastewater. This work involved the preparation of a CoCN0.02 photocatalyst by simple thermal polymerization. The synthesized catalysts were mainly used for the photocatalytic degradation of tetracycline (TC) pollutants. The photocatalytic efficiency of one of the catalysts reached 97% in 30 min, which was much higher than that of pure g-C3N4 (CN). The consistency between the results of kinetic simulations and characterization supported the strong role of Co intercalation sites in photocatalysis. Additionally, using the active species capture experiments, the predominant active species were determined to be •OH, •O2−, and h+, thereby allowing us to explore the electron transportation and redox reactions during the process of photocatalysis. This investigation establishes a basis for exploring the evolution of active species in the context of antibiotic pollutants.

The inadequate biosafety of MRI contrast agents (CAs) remains a challenging issue. Both increasing the magnetic relaxivity of CAs and targeting them through conjugation with folates are promising approaches to addressing this issue. Silica nanoparticles (SNs) with Mn2+ ions specifically localized in the outer layer were selected as the target for further surface modification for the covalent attachment of folates. It was shown that when Mn-containing SNs are conjugated with folates via preliminary amino modification of the surface silanol groups, the folate-conjugated SNs suffer from colloidal instability. Thus, precoating Mn-containing SNs with unfolded BSA exposes surface amino groups that successfully conjugate with folates without loss of colloidal stability. Partial washout of surface-localized Mn2+ follows folate conjugation of Mn-containing SNs, although residual Mn2+ ions provide r1(2) relaxivities of 62.1 (160.4) mM−1s−1 at 0.47 T.

The present work demonstrates the optimization of the ligand structure in the series of bis(phosphine oxide) and β-ketophosphine oxide representatives for efficient coordination of Tb3+ and Eu3+ ions with the formation of the complexes exhibiting high Tb3+- and Eu3+-centered luminescence. The analysis of the stoichiometry and structure of the lanthanide complexes obtained using the XRD method reveals the great impact of the bridging group nature between two phosphine oxide moieties on the coordination mode of the ligands with Tb3+ and Eu3+ ions. The bridging imido-group facilitates the deprotonation of the imido- bis(phosphine oxide) ligand followed by the formation of tris-complexes. The spectral and PXRD analysis of the separated colloids indicates that the high stability of the tris-complexes provides their safe conversion into polystyrenesulfonate-stabilized colloids using the solvent exchange method. The red Eu3+-centered luminescence of the tris-complex exhibits the same specificity in the solutions and the colloids. The pronounced luminescent response on the antibiotic ceftriaxone allows for sensing the latter in aqueous solutions with an LOD value equal to 0.974 μM.