Liping Guo

Constructing single-atom transition-metal-implanted mesoporous metal–organic frameworks (MOFs) for CO2 conversion is of great importance for achieving carbon neutrality, yet remains a formidable challenge. This work presents a modular optimization of cerium-based metal–organic frameworks by incorporating Co single atoms with ordered mesopores (OMCU). These periodically arranged mesopores in OMCU were fabricated by synergistically combining the Hofmeister effect with a soft-template structure-oriented strategy. Mechanistic investigations reveal that the Co single atoms could not only accelerate photogenerated electron participation in CO2 conversion but also lower the energy barrier by promoting the formation of a new intermediate, *OCHO, along a specific reduction pathway, as directly observed by in situ Raman and operando ATR-IR spectroscopy. Density functional theory calculations corroborate that Co atoms favor the generation of *OCHO-related intermediates, omitting the high energy input for CO2·– formation and resulting in outstanding CO2 reduction performance, which is equivalent to a 10.84-fold enhancement in CO generation rate compared to that of the pristine MOF in the presence of TEA and bipyridinium ruthenium. This work provides an effective strategy through the construction of active cobalt sites within ordered mesoporous cerium-based MOFs for modulating the key intermediates in CO2 photoreduction.

The electrooxidation of amines to nitriles (AOR) offers a promising alternative to the oxygen evolution reaction (OER) for energy-saving hydrogen production coupled with value-added synthesis. However, simultaneously achieving high activity, selectivity, and OER suppression remains a key challenge. Herein, we demonstrate a multistrategy optimization approach for efficient propylamine electrooxidation reaction by synergistically tailoring catalyst properties and electrolyte composition. We first develop a Mo-doped Ni3S2 electrocatalyst (Mo-Ni3S2), where Mo doping performs dual functions: electronically modulating Ni sites to generate high-valence active centers for dehydrogenation and inducing the generation of surface SO42− groups. These groups create a negatively charged interface that enriches amine reactants while repelling hydroxyl species, thereby suppressing OER. As a second important strategy, the electrolyte (0.4 M KOH + 0.1 M Na2SO4) was engineered to effectively suppress product hydrolysis. This integrated approach enables the optimized system to deliver exceptional performance: ultrahigh activity (Tafel slope of 20.9 mV dec−1), ≥97% Faradaic efficiency for propionitrile at 90 mA cm−2, and high reaction selectivity. When coupled with the hydrogen evolution reaction (HER) in a two-electrode system, the AOR||HER electrolyzer requires only 1.42 V to reach 10 mA·cm−2 (vs 1.63 V for OER||HER); in an H-cell at 90 mA·cm−2, the H2 Faradaic efficiency remains 98−99%, while the propionitrile FE decreases from 95% at 1.45 V to 80% at 1.65 V, establishing a viable paradigm for coproducing hydrogen and valuable nitriles.

The catalytic conversion of CO ₂ into industrially relevant chemicals offers a sustainable pathway for carbon mitigation, yet most existing methods require harsh reaction conditions. In this work, a series of substituted cobalt (II) dibenzoylmethane complexes (Co(x‐dbm) ₂ ) were applied to enable efficient CO ₂ fixation with epoxides or aziridines at ambient pressure. Systematic substituent screening demonstrated that electron‐donating groups (CH ₃ , t‐Bu) significantly enhanced the catalytic activity in both CO ₂ /epoxide and CO ₂ /aziridine systems. For epoxide coupling, the optimized catalyst achieves up to 96% epoxide conversion and > 99% selectivity for cyclic carbonates at 40°C with only 0.5 mol% catalyst loading. Parallel experiments highlighted that electron‐donating substituents simultaneously strengthen metal–ligand coordination and improve solubility, synergistically boosting catalytic efficiency. For aziridine coupling, 63% aziridine conversion with 92% oxazolidinone selectivity was attained at 40°C using tetrabutylammonium bromide (TBAB) as cocatalyst, whereas 86% aziridine conversion and 87% selectivity were achieved at 80°C with tetrabutylammonium chloride (TBAC) as cocatalyst. The balance between nucleophilicity (driving aziridine ring‐opening) and leaving‐group ability (facilitating ring‐closure of the intermediate carbamate salt to form the oxazolidinone) of the halide anions (XCl, Br, I) in tetrabutylammonium cocatalysts (TBAX) influenced both activity and selectivity, demonstrating the comparable rates of the ring‐opening and ring‐closing steps.

The Fe₃O₄@SiO₂@MOF can detect the concentration of 4-nitrophenol within 30 s, and has a good linear relationship with 4-nitrophenol in the concentration range of 5–200 μM (R² = 0.9946), and the detection limit is 2.2 μM (S/N = 3).

In this work, CoV-LDH/ZnIn₂S₄ (CoV-LDH/ZIS) nanocomposites were synthesized through a self-assembly process in order to investigate the influence of CoV-LDH addition on the rate of hydrogen production. XRD and TEM measurements confirmed the effective preparation of CoV-LDH/ZIS nanocomposites. Among all the nanocomposite photocatalysts, 2.0%-CoV-LDH/ZIS showed the best photocatalytic performance with a hydrogen production rate of 1397.3 μmol g⁻¹ h⁻¹, approximately 2.2 times that of pure ZnIn₂S₄ (ZIS). The X-ray photoelectron spectroscopy (XPS) measurement indicated that there is a strong interfacial interaction between ZIS and CoV-LDH, indicating that more than simple mechanical mixing had occurred. The steady-state fluorescence spectroscopy (PL) and time-resolved photoluminescence (TRPL) spectroscopy results showed that the electron and hole recombination in CoV-LDH/ZIS is significantly reduced and that efficient interface charge transfer and separation are achieved. This work sheds light on the interfacial electron transfer between two semiconductor materials, which promotes the separation of photogenerated carriers and thus enhances photocatalytic hydrogen production activity.

A magnetic, mesoporous core/shell structured Fe₃O₄@SiO₂@mSiO₂ nanocomposite was synthesized and employed as a magnetic solid phase extraction (MSPE) sorbent for the determination of trace sulfonamides (SAs) in food samples. The synthesized nanocomposite was characterized by transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, X-ray diffraction, N₂ sorption analysis and vibrating sample magnetometry. The results showed that Fe₃O₄@SiO₂@mSiO₂ possessed a mesoporous structure with a large surface area. Batch experiments were carried out to investigate the adsorption ability for SAs. Fe₃O₄@SiO₂@mSiO₂ showed fast kinetics and high adsorption capacity, and the pseudo-second-order model and Langmuir adsorption isotherm are well fitted with the experimental data, indicating that chemical adsorption might be the rate-limiting step. Moreover, the high adsorption capacity can be maintained for at least 8 runs, indicating excellent stability and reusability. The proposed method exhibited good linearity in the range of 0.2–500 μg L⁻¹, the R² values of all the analytes were greater than 0.99 and the LODs were all lower than 0.2 μg L⁻¹. Furthermore, real food samples were successfully analyzed with Fe₃O₄@SiO₂@mSiO₂ and high recoveries varying from 89.7% and 110.6% were obtained with low relative standard deviations ranging from 1.78% to 6.91%. The Fe₃O₄@SiO₂@mSiO₂ magnetic nanocomposite is a promising sorbent for the efficient extraction of SAs from complex food samples.

The synthesis of cyclic carbonates from epoxides and carbon dioxide using metal-free catalyst systems is critically reviewed.

NiS ₂ nanoparticles (NPs)‐modified CdS nanowires (NWs) (NiS ₂ /CdS) with varying amount of NiS ₂ were synthesized via a two‐step approach and characterized for sustainable hydrogen evolution. They showed much higher activity than pristine CdS NWs or NiS ₂ NPs, with the optimal hydrogen production rate reaching 14.49 mmol⋅h ⁻¹ ⋅g ⁻¹ for 40%‐NiS ₂ /CdS with lactic acid as sacrificial agent. Under optimal conditions, hydrogen generation rate of 52.88 μmol⋅h ⁻¹ ⋅g ⁻¹ was achieved using single cellulose as sacrificial agent. Photoelectrochemical (PEC) properties of the NiS ₂ /CdS nanocomposites were investigated to gain a better understanding of the mechanism behind the enhanced photocatalytic hydrogen evolution reaction (HER) activity. Furthermore, ultrafast transient absorption (TA) spectroscopy was also employed to investigate the charge carrier dynamics, revealing an exciton lifetime approximately four times shorter in 40%‐NiS ₂ /CdS nanocomposite compared to pristine CdS NWs. These results suggest efficient charge transfer from CdS to NiS ₂ . A possible mechanism for enhanced hydrogen production over NiS ₂ /CdS nanocomposite is proposed.

Metal β-diketonate complexes could efficiently catalyze the chemical fixation of CO₂ at 1 atm and near room temperature.