Molecular Catalysis
·
2024
·
IF 3.9
Zheng Zhou,Meng Miao,Wenzhi Li,Jingting Jin,Liqun Wang,Lulu Zhang,Liang Yuan
The selective conversion of methane is a significant but difficult challenge. We reported a CuFe bimetallic catalyst supported by g-C 3 N 4 for the catalytic oxidation of methane to oxygenated C1 products. Using H 2 O 2 as the oxidant, Cu 0.4 Fe 0.3 -C 3 N 4 catalyst had a C1 yield of 8231 μmol·g cat −1 · h −1 at 70 °C, and 1 H NMR results showed that almost all of the liquid phase products were target C1 products. The methanol selectivity on CuFe-C 3 N 4 was 44.5 %, comparing with 20.2 % methanol selectivity on Cu-C 3 N 4 . The formation of a Cu-O-Fe site on the CuFe-C 3 N 4 was confirmed by in situ DRIFTS and 57 Fe Mössbauer spectroscopy. This Cu-O-Fe site was responsible for the improved catalyst performance. DFT calculations illustrated that at the Cu-O-Fe site, H 2 O 2 dissociated into two ·OH radicals instead of ·H and ·OOH radicals as it did at the Cu-O-Cu site. The ·OH radicals combined with the ·CH 3 radicals from the CH 4 molecules to form methanol. These findings provided valuable insights into the rational design of active sites on carbon nitride materials.
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Chemosensors
·
2025
·Vol. 13
·期 3
·81
·
IF 3.7
Peizheng Shi,Ningbin Zhao,Zhuang Sun,Kaiqiang Sun,Wubo Chu,Hsu-Sheng Tsai,Lidong Wu,Tao Cai,Yuezhong Wang,Nan Jiang,Chen Ye,Li Fu,Lixin Xu,Cheng-Te Lin
Uric acid (UA), the final metabolic product of purines, plays a crucial role in human health monitoring. The UA concentration in biological fluids serves as a diagnostic marker for various disorders, particularly kidney diseases, and represents a potential therapeutic target. Given the growing emphasis on preventive healthcare, developing methods for real-time UA detection has become increasingly significant. Here, we demonstrate the synthesis of novel tumbleweed-like molybdenum diselenide (MoSe2) nanostructures through a single-step hydrothermal process. The synthesized MoSe2was subsequently hybridized with reduced graphene oxide (rGO) to construct electrodes for UA sensing. Differential pulse voltammetry (DPV) measurements revealed that the MoSe2/rGO-modified glassy carbon electrode (GCE) exhibited excellent UA detection capabilities under optimized conditions. The sensor demonstrated a remarkably low limit of detection (LOD) of 28.4 nM and maintained linearity across a wide concentration range (40 nM to 200 μM). Notably, the sensor showed high selectivity for UA detection even in the presence of common interfering species, including citric acid (CA), dopamine (DA), ascorbic acid (AA), cysteine (Cys), glucose (Glu), oxalic acid (OA), sodium ions (Na+), and potassium ions (K+). The developed sensor displayed outstanding selectivity, stability, and reproducibility characteristics. This synthetic approach offers promising opportunities for developing MoSe2-based electrochemical sensing platforms suitable for diverse bioanalytical applications.
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Crystals
·
2024
·Vol. 14
·期 10
·896
·
IF 2.4
Wenfang Zhou,Zirui Wang,Qingfeng Wu,Qinping Nie,Yi Wang
Suspended particulate matter (SPM) is an important component of natural water bodies and can significantly influence the photolytic behavior of water pollutants. A comprehensive understanding of the photochemical behavior of water pollutants in natural waters requires consideration of the presence of SPM. In this study, montmorillonite–humic acid (MMT-HA) composite particles were synthesized to simulate SPM in natural waters and their effects on the photolysis of tetracycline (TC) were investigated. The results demonstrated that the presence of MMT-HA composite particles in water significantly enhanced the photolysis of TC, with the photolytic kinetics following a pseudo-first-order model. Electron spin resonance spectra and free radical quenching experiments indicated that the photoactive components (MMT and humic acids) in the composite particles induced the generation of reactive oxygen species under light exposure, further contributing to the enhanced photolysis of TC. Comparative analysis of the free radical signals and adsorption experiments revealed that the accelerated photolysis of TC was also related to the interfacial interaction between the MMT in the composite particles and the TC molecules. The formation of surface complexes between TC molecules and the negatively charged sites on the MMT surface facilitated light absorption and electron transfer, thereby accelerating the photolysis of TC. Photoproduct analysis indicated that the primary degradation pathways of TC in the composite particle systems included the addition of hydroxyl radicals to the aromatic ring, as well as demethylation, deamination and dehydration in the side chains. This study shows that SPM in water bodies can affect the photochemical behavior of pollutants and should be taken into account when assessing the phototransformation of pollutants in natural waters.
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CHEMOSPHERE
·
2024
·
IF 8.1
Yaxi Deng,Hongxia Zhao,Xiaonuo Zhang,Xintong Li,Goujian Chi
Complex rhizoremediation is the main mechanism of phytoremediation in organic-contaminated soil. Low molecular weight organic acids (LMWOAs) in root exudates have been shown to increase the bioavailability of contaminants and are essential for promoting the dissipation of contaminants. The effects of root exudates on the dissipation of organophosphate esters (OPEs) in soil are unclear. Consequently, we studied the combined effects of root exudates, soil enzymes and microorganisms on OPEs (tri (1-chloro-2-propyl) phosphate (TCPP) and triphenyl phosphate (TPP)) dissipation through pot experiments. Oxalic acid (OA) was confirmed to be the main component of LMWOAs in root exudates of ryegrass. The existence of OA increased the dissipation rate of OPEs by 6.04%–25.50%. Catalase and dehydrogenase activities were firstly activated and then inhibited in soil. While, urease activity was activated and alkaline phosphatase activity was inhibited during the exposure period. More bacteria enrichment (e.g., Sphingomonas , Pseudomonas , Flavisolibacter , Pontibacter , Methylophilus and Massilia ) improved the biodegradation of OPEs. In addition, the transformation paths of OPEs hydrolysis and methylation under the action of root exudates were observed. This study provided theoretical insights into reducing the pollution risk of OPEs in the soil.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Siyi Pan,Pingxiao Wu,Leiye Sun,Meiqing Chen,Bo Li,Tianming Wang,Zhongbo Shang,Jiangmin Fang,Nengwu Zhu,Zhi Dang
Green rust (GR), as a vital intermediate product during the formation of various iron oxides, exists with organic matters and metals contaminants in natural environments. Understanding the effects of these natural factors on the transformation process of GR into iron oxides and the environmental behaviors of heavy metals and organic matters during process are critical for environmental quality management, but the fundamental identification of the interaction mechanisms between them and GR is still challenging. In this study, the transformation mechanisms of Co-bearing green rust (GR-Co) synthesized by co-precipitation, and the redistribution behaviors of Co(II) in an environment containing oxalic acid (OA) and citric acid (CA) were clarified. The findings indicated that OA promoted the Fe(II) dissolution and the transformation of GR-Co to goethite, while CA decreased the Fe(II) dissolution and the proportion of non-extractable Co. Furthermore, in the presence of CA, the transformation products of GR-Co were ferrihydrite, magnetite, lepidocrocite and goethite instead of only lepidocrocite and goethite. Meanwhile, CA prohibited ferrihydrite from transforming into more highly crystalline iron minerals. The finding of this study improves the understanding of the interaction mechanisms between GR-Co and organic matter, and the environmental geochemical behaviors of Co and organic carbon during the transformation processes in nature.
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CHEMOSPHERE
·
2024
·
IF 8.1
Dan Zhou,Chao Li,Mingzheng Huang,Xiaoyan Chen,Yonglian Xia,Yi Huang
V–Ti magnetite tailings (VTMTs) contain various heavy metals , such as Fe, Mn, V, Co, and Ni. The groundwater pollution caused by the tailing metal release has become a local environmental concern. Although studies have demonstrated the influence of alternate flooding and drying cycles (FDCs) on metal form and mobility in minerals, little was known about whether FDCs affect the metal release of VTMTs and the transformation of released metals. This study investigated the metal release kinetics of VTMTs and the metal transformation under FDCs in the absence and presence of acid rain (sulfuric and nitric acids) and bio-secreted organic acids (acetic, oxalic, and citric acids). The results showed that FDCs promoted metal release whether or not acids were present. The maximum released concentrations of V, Mn, Fe, Co, and Ni were as high as 78.63 mg L −1 ,1.47 mg L −1 , 67.96 μg L −1 , 1.34 mg L −1 , and 0.80 mg L −1 , respectively, under FDCs and citric acids . FDCs enhanced the tailing metal release by increasing the metal labile fraction proportion. However, the concentrations of released Fe, Mn, V, Co, and Ni all gradually decreased due to their (co-)precipitation. These precipitates conversely inhibited the subsequent mineral dissolution by covering the tailing surface. FDCs also enhanced the tailings’ porosities by 2.94%–9.94%. The mineral dissolution, expansion and shrinkage, and changes in tension destroyed the tailing microstructure during FDCs. This study demonstrated the low metal pollution risk of VTMTs under FDCs, either in acid rain or bio-secreted organic acids. However, the increase in tailing porosity should be seriously considered as it would affect the tailing pond safety.
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ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Guozhen He,Tao Dong,Zhaochu Yang,Bjo̷rn Torger Stokke,Zhuangde Jiang
Biofouling deteriorates the performance of sensors operated in biofluids. Protein adsorption is believed to be the first step of biofouling, which also reduces biocompatibility by further inducing cell adhesion, platelet activation, and even inflammation. Current studies of antifouling coatings are focused on polymers and hydrogels, which have succeeded in remaining resistant to protein adsorption, but their application on sensor electrodes is limited due to low conductivity and biocompatibility. Here, we report a spontaneous antibiofouling strategy for sensor electrodes by controlling oxygen vacancies in WO3 nanosheets. Irreversible adsorption of proteins was reduced by 76% in unprocessed human plasma when electrodes were coated with WO3 rich in surface oxygen vacancy. These electrodes maintained 91% of the initial current density after 1 month of incubation in human plasma.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Changshun Deng,Xiaorong Zhu,Jun Yao,Yibo Wang,Chenyang Shen,Bingqing Ge,Chaoxiang Li,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Yafei Li,Weiping Ding
The direct oxidation of toluene by O 2 to benzaldehyde with high efficiency is a bright route for the green production of benzaldehyde but still a significant challenge. In this study, we develop a ligand modification strategy by bonding organophosphonic acid (OPA) to VTiO x /γ-Al 2 O 3 to restructure its interface microenvironment for enhancement of toluene oxidation to benzaldehyde. The as-prepared catalyst exhibits excellent selectivity over 99 % under mild conditions. Results of comprehensive characterizations and calculations reveal that the OPA bonding in bidentate with the V 6-coordinated species causes noticeable phase reconstruction between VO x and TiO 2 , thereby generating nearby new reactive oxygen species, which is responsible for the conversion of toluene to benzaldehyde at temperatures as low as ∼50 °C, much lower than that over VO x /TiO 2 (>130°C). The interface microdomain around the bonding site of OPA helps to significantly weaken the methyl C H bond of toluene molecule in reaction manifested as the significant decrease in apparent activation energy. Hence, the current work reveals a novel mechanism of the typical catalyst VO x /TiO 2 under OPA bonding, which is useful to solve the classic difficult reaction of toluene to benzaldehyde by O 2 oxidation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Junjie Jiang,Yongqi Zhao,Xue Li,Xiaolong Liu,Tingyu Zhu
Nitrogen oxides (NO x ) and volatile organic compounds (VOCs) released from industrial sources react to generate pollutants such as O 3 through photochemical reactions. In order to realize the simultaneous removal of NO x and VOCs, this work provides a reaction site-isolation (RSI) catalyst with isolated reaction zones of toluene oxidation over Cu-Ce sites and NH 3 -SCR over V-W sites, respectively. Reaction site-isolation significantly weakens the impact of competitive adsorption between different reactants and reduces the formation of by-products during the reaction. The NO and toluene conversion both reached to 100 % at 275 ℃ and the catalyst demonstrated great sulfur resistance and stability. Characterization of the catalyst revealed that the interaction between Cu and Ce promoted the formation of oxygen vacancies, while the introduction of Cu increased the adsorption sites of toluene. Notably, DFT calculation and activation energy calculation reveal that the adsorption performance of active sites for reactant and the reaction activation energy required for reactions are different. Therefore, this work achieves adsorption and reaction co-induced bifunctional catalysis by isolating active sites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Hongfan Huang,Haihui Wu,Jiqing Zhang,Tao Zou,Ende Feng,Xuekun Sui,Wenjing Zhang,Bao Liu,Liu Yang,Xiaohui Guan,Penggang Yin,Guangsheng Wang
Exploiting high-quality cathode materials and optimizing their electrochemical performance for aqueous zinc-ion batteries (AZIBs) is of prominent significance for the advancement of charge storage devices. Herein, a novel zeolitic imidazolate framework assisted synthesis method has been proposed for the first time to prepare C and N co-doped Mn 2 O 3 /Co 3 O 4 cathode (C/N-Mn 2 O 3 /Co 3 O 4 ) with unique hollow hexahedron structure. Theoretical, simulative, and experimental results all reveal that primarily benefiting from synergistic effects, the drawbacks of low structural stability and electrical conductivity for Mn 2 O 3 , and the shortcomings of inferior electrochemical activity and cycling stability for amorphous Co x O y (A-Co x O y ), could be effectively compensated. In addition, the unique hollow hexahedron structure could provide abundant active sites and electron transfer paths, which is conducive to the enhancement of electrochemical activity and kinetics. The zinc battery utilizing C/N-Mn 2 O 3 /Co 3 O 4 as cathode exhibits a high specific capacity of 355.9 mAh·g −1 at 0.1 A·g −1 , which is much higher than that of A-Co x O y . After dozens of cycling at different current densities, the specific capacity could be retained, indicating superior rate performance. Moreover, the specific capacity presents no decrease during initial 600 repeated charge/discharge cycles, suggesting admirable cycling stability. Additionally, the electrochemical kinetics and energy density of the AZIBs are also distinctly improved.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yuzhi Liu,Chuang Wu,Wei Gao,Shuang Zhong,Wenbing Zhao,Shuai Xia,Haiyang Yu,Nan Shao,Yu Gao,Donglei Zou
Tailwater treatment from high-standard plastic-cleaning wastewater and red mud (RM) resource recycling pose major challenges. In this study, a heterogeneous microwave-responsive catalyst, RM/biochar (RM/BC), was successfully prepared to synergistically integrate magnetic and dielectric losses for activation of sodium percarbonate (SPC) to degrade the plastic additive diethyl phthalate (DEP). Characterization analyses revealed that under oxygen-limited conditions at 600 °C, poplar leaf powder was fully carbonized, while Fe 2 O 3 in RM was reduced to FeO and further transformed into Fe 3 O 4 , forming a composite dominated by amorphous carbon and Fe 3 O 4 . In RM/BC-600, Fe 3 O 4 and amorphous carbon collaboratively enabled dual hot-spot effects under microwave irradiation via magnetic and dielectric losses, accompanied by enriched oxygen vacancies. Hydroxyl radicals (•OH) were identified as the dominant reactive oxygen species (ROS) in SPC activation. Through single-factor and response surface optimization, under conditions of 40 μM DEP concentration, 4.03 mM SPC dosage, 6.24 g/L RM/BC-600 dosage, 87.2 °C reaction temperature, and 100 W microwave power, the optimal DEP removal efficiency reached 96.1 %. In-situ FTIR/Raman spectroscopy and EPR analysis demonstrated that RM/BC primarily facilitated SPC decomposition to hydrogen peroxide, with oxygen vacancies catalyzing hydrogen peroxide to generate •OH as the main ROS, supplemented by carbonate radicals (•CO 3 − ), superoxide radicals (•O 2 − ), and singlet oxygen ( 1 O 2 ), while dual hot-spot effects accelerated this process. HPLC-QTOF-MS identified 12 intermediate products, and plausible degradation pathways were proposed. ECOSAR software predicted reduced acute toxicity of degradation products, and seed germination assays confirmed minimal ecotoxicity of RM/BC to soil-plant systems. This study achieves RM resource recovery and hazard mitigation via a green strategy, enhancing plastic wastewater treatment through DEP detoxification and stability.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Jie Chen,Ruilan Li,Yongzhi Duan,Shuaiqi Gong,Yulin Min,Hexing Li,Penghui Shi
The cyclic regeneration of non-renewable graphite anode materials in lithium-ion batteries (LIBs) is crucial for battery recycling, aiming to reduce carbon footprints and minimize resource waste. Traditional methods often involve high energy use and significant environmental pollution. To tackle this, a green, closed-loop regeneration method using only oxalic acid was developed. This approach efficiently recovers precious metals from the anode and allows for in-situ regeneration of the spent anode, as well as the synthesis of pre-lithiation reagents. The findings indicate that lithium oxalate on the surface of pre-lithiated regenerated graphite compensates for active Li+ loss and acts as a pre-lithiation sacrificial salt during battery operation. It also decomposes to release carbon dioxide, preventing the formation of soluble lithium alkoxides and electrolyte ester exchange reactions, significantly enhancing battery performance without leaving impurities. This method allows effective lithium utilization from spent anodes and in-situ closed-loop regeneration. Under optimal conditions, the Li+ leaching rate reaches 97.64%. The electrochemical performance of the regenerated prelithiated graphite maintains a high specific capacity of 320.5 mAh·g−1 after 200 cycles, with a specific capacity retention rate of 90.4%. Environmental and economic assessment shows outstanding economic advantages of $3,259.22 and negligible environmental footprint for recycling each 1.0 ton of retired graphite. This work advances material recycling, reduces the environmental impact of waste batteries, and supports a low-carbon transition.
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