APPLIED SURFACE SCIENCE
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2024
·
IF 6.3
Haiyang Xie,Tianyi Guo,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Tao Gan
Modulating the coordination structure of active center atoms of atomically dispersed metal catalysts has emerged as a critical strategy to further enhance the catalytic performance for selective hydrogenation. Herein, we report the successful synthesis of atomically dispersed cobalt catalysts supported on N, P co-doped cellulose-derived carbon (Co 1 /NPC) via a mechanical activation assisted synthesis method. The introduction of P and N atoms modifies the electronic structure of Co atoms by forming Co–N x and Co–P x structures, enhancing their ability to dissociate H 2 and adsorb nitroarenes, thereby significantly boosting the hydrogenation activity. Consequently, the Co 1 /NPC catalyst demonstrates outstanding catalytic activity for the selective hydrogenation of nitrobenzene, achieving 99 % conversion and selectivity with a high TOF of 507 h −1 , far outperforming the benchmark Co 1 /NC (TOF of 4 h −1 ) and Co NPs /NPC catalysts (TOF of 10 h −1 ). Moreover, Co 1 /NPC catalysts possess exceptional stability and satisfactory universality. This study provides an efficient and practical catalyst for the production of nitroanilines via the selective hydrogenation of nitroarenes.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Dingfeng Yang,Hongzheng Pu,Peng Dai,Wen Jiang,Yuanxue Yi,Tao Zhang,Shuming Zhang,Xichuan Guo,Yuanyuan Li
A systematic evaluation of enhancing photocatalysis via aliovalent cation doping is conducted. Cation In3+, being p-type-doped, was chosen to substitute the Sn site (Sn4+) in Li2SnO3, and the photodegradation of 2,4-dichlorophenol was applied as a model reaction. Specifically, Li2Sn0.90In0.10O3 exhibited superior catalytic performance; the photodegradation efficiency reached about 100% within only 12 min. This efficiency is far greater than that of pure Li2SnO3 under identical conditions. Density functional theory calculations reveal that introducing In3+ increased the electron mobility, yet decreased the hole mobility, leading to photogenerated carrier separation. However, photoluminescence and time-resolved photoluminescence suggest that In3+ induced nonradiative coupling in the matrix, reducing the photogenerated carrier separation ratio compared with that of Li2SnO3. The optical band gap of Li2Sn0.90In0.10O3 was almost unchanged compared with that of Li2SnO3 via ultraviolet–visible absorption. The increased photocatalytic efficiency was ascribed to the lower valence band position and enhanced hole concentrations by valence band X-ray photoelectron spectroscopy and electrochemical measurements. Finally, a 2,4-dichlorophenol degradation pathway, an intermediate toxicity assessment, and a photocatalytic mechanism were proposed. This work offers insights into designing and optimizing semiconductor photocatalysts with high performance.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
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IF 8.1
Yining Bao,Qingru Zeng,Shunyan Ning,Wei Zhao,Longfei Wang,Xinpeng Wang,Yuezhou Wei,Deqian Zeng
Developing effective heterojunction photocatalysts that efficiently separate charge carriers and improve light-harvesting capabilities is crucial in addressing energy and environmental issues. Herein, a unique nanocomposite photocatalyst is constructed by attaching CoMn 2 O 4 nanoparticles onto 2D CdS nanosheets for H 2 production and U(VI) reduction. The optimized 2% CoMn 2 O 4 /CdS nanocomposite showcases the highest photocatalytic H 2 production efficiency, 5.8 times higher than CdS nanosheets . Additionally, the U(VI) reduction rate constant of 2% CoMn 2 O 4 /CdS is 0.0192 min −1 , approximately 1.9 folds over the pristine CdS (0.0101 min −1 ). The exceptional photocatalytic performance toward photocatalytic H 2 evolution and U(VI) reduction reactions directly result from the electronic integration between CoMn 2 O 4 /CdS p-n heterojunction, facilitated by the efficient photoexcited charge separation. Feasible photocatalytic mechanisms are proposed through experimental analyses and theoretical calculations. This study provides a straightforward method for designing effective CdS-based heterostructured photocatalysts, contributing to the advancement of solar-to-H 2 conversion and environmental abetment.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 6
·1-11
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IF 5.3
Kong Qingfei,Liu Chunhan,Zhang Yanlin,He Yifan,Zhang Ruiting,Wang Yuhan,Zhou Qin,Cui Feiyun
The instant screening of patients with a tendency towards developing Alzheimer’s disease (AD) is significant for providing preventive measures and treatment. However, the current imaging-based technology cannot meet the requirements in the early stage. Developing biosensor-based liquid biopsy technology could be overcoming this bottleneck problem. Herein, we developed a simple, low-cost, and sensitive electrochemical aptamer biosensor for detecting phosphorylated tau protein threonine 231 (P-tau231), the earliest and one of the most efficacious abnormally elevated biomarkers of AD. Gold nanoparticles (AuNPs) were electrochemically synthesized on a glassy carbon electrode as the transducer, exhibiting excellent conductivity, and were applied to amplify the electrochemical signal. A nucleic acid aptamer was designed as the receptor to capture the P-tau231 protein, specifically through the formation of an aptamer-antigen complex. The proposed biosensor showed excellent sensitivity in detecting P-tau 231, with a broad linear detection range from 10 to 10 7 pg/mL and a limit of detection (LOD) of 2.31 pg/mL. The recoveries of the biosensor in human serum ranged from 97.59 to 103.26%, demonstrating that the biosensor could be used in complex practical samples. In addition, the results showed that the developed biosensor has good repeatability, reproducibility, and stability, which provides a novel method for the early screening of AD. Graphical Abstract
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ANALYTICA CHIMICA ACTA
·
2024
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IF 5.7
Caiming Tang,Yizhe Zhu,Ruifen Zheng,Ling Liu,Yan-Hong Zeng,Xiao-Jun Luo,Bi-Xian Mai
Background N,N′-disubstituted p -phenylenediamine-quinones (PPDQs) are oxidization derivatives of p -phenylenediamines (PPDs) and have raised extensive concerns recently, due to their toxicities and prevalence in the environment, particularly in water environment. PPDQs are derived from tire rubbers, in which other PPD oxidization products besides reported PPDQs may also exist, e.g., unknown PPDQs and PPD-phenols (PPDPs). Results This study implemented nontarget analysis and profiling for PPDQ/Ps in aged tire rubbers using liquid chromatography-high-resolution mass spectrometry and a species-specific algorithm. The algorithm took into account the ionization behaviors of PPDQ/Ps in both positive and negative electrospray ionization, and their specific carbon isotopologue distributions. A total of 47 formulas of PPDQ/Ps were found and elucidated with tentative or accurate structures, including 25 PPDQs, 18 PPDPs and 4 PPD-hydroxy-quinones (PPDHQs). The semiquantified total concentrations of PPDQ/Ps were 14.08–30.62 μg/g, and the concentrations followed the order as: PPDPs (6.48–17.39) > PPDQs (5.86–12.14) > PPDHQs (0.16–1.35 μg/g). Significance The high concentrations and potential toxicities indicate that these PPDQ/Ps could seriously threaten the eco-environment, as they may finally enter the environment, accordingly requiring further investigation. The analysis strategy and data-processing algorithm can be extended to nontarget analysis for other zwitterionic pollutants, and the analysis results provide new understandings on the environmental occurrence of PPDQ/Ps from source and overall perspectives.
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ENERGY & FUELS
·
2018
·
IF 3.024
Qian Zhao,Wenbo Zhao,Muyuan Chai,Ling Chen,Yang Wang,Qingming Jia,Yuan Chen
As SO2 removal via traditional aqueous amine scrubbing requires large amounts of energy for absorbent regeneration, phase-change absorption was considered to be a promising alternative, as regeneration of only the SO2-rich phase is needed. The SO2-lean phase can be directly reused, thus greatly reducing energy requirements. We herein investigated the phase-change absorption behavior of N,N,N′,N′-tetramethyl-p-phenylenediamine (TPD) in organic solvents. In general, the TPD absorption rate in organic solvents followed the order: dimethylformamide > diethylene glycol dimethyl ether > propylene carbonate > butanol, which is related to their Henry’s constant. Our results indicated that TPD reacted with SO2 to form the charge-transfer complex TPD·SO2, which was further converted into TPD·2SO2 upon increasing the absorption time. Furthermore, the addition of H2O promoted the formation of TPD·2SO2, but it exhibited a negative effect on the absorption rate. Moreover, in the presence of O2 and H2O, TPD·SO2 in solution was converted slowly into [H2TPD][HSO4]2. TPD·SO2 decomposed into TPD and SO2 at ∼100 °C and exhibited a relatively stable recyclability for SO2 absorption. At last, TPD·SO2 was used as a surrogate of SO2 to synthesize sulfonamide; its activity was higher than that of a reported complex of triethylenediamine and SO2.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Qianfeng Wu,Binbin Tan,Jiang Wang,Zhihao Zhang,Jing Wang,Junlong Liu,Yao Deng,Huidi Zhang,Ting Yang,Wenlei Wang
The utilization of a low-cost common waste biomass, mugwort, with a porous structure is important for the treatment of Arsenic (III) pollution in the aquatic environment. In this study, mugwort straw was first delignified to expose more hydroxyl groups, then loaded with MnOOH and α − FeOOH and constructed with p − n heterojunctions on cellulosic biochar microinterfaces. The successful formation of p − n heterojunction effectively enhances the electric field enhancement inside the photocatalyst, promotes charge transfer and suppresses the recombination of photogenerated carriers. Application of high-energy electron beam irradiation of FMBC−LR2 to modulate the generation and dominant mechanism of Fe and Mn in the reaction system. The results showed that Mn 3+ underwent disproportionation reaction to form Mn 2+ and Mn 4+ . Among them, Mn 2+ led to the formation of MnFe 2 O 4 , while Mn 4+ exhibited stronger oxidizing properties that could promote the transformation of Fe 2+ to Fe 3+ , thus allowing more Fe 3+ to participate in the photocatalytic oxidation of As(III) in a synergistic manner. As(III) oxidation efficiency increased 9.18 times after delignification treatment (FMBC−LR2) and 12.31 times after high-energy electron beam irradiation (FMBC−LR2 − 650) as compared to mugwort straw biochar (BC). In addition, the EPR assay results indicated that ·O 2 − , ·OH, and 1 O 2 acted together in the As(III) reaction. This provides new insights into the remediation of composite modified biochar in water bodies and a new environmentally friendly strategy for the comprehensive utilization of straw materials.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jialin Li,Yu Wang,Ye Zhang,Wei Zhao,Wenzhe Bao,Yufeifan Duan,Junwei Yu,Bo Zhu,Kun Qiao
Currently, the hydrogen storage application of carbon-based adsorbent materials is mostly implemented under the pressure conditions of 30–300 bar, while there is few targeted studies conducted on the unsaturated adsorption under ambient pressure conditions. Therefore, based on industrialized Lyocell biopolymer fiber precursors and the enhancement effects of dipole-induced hydrogen bonds (DIHB), this work presents a facile construction strategy for P/O co-doped Lyocell-based porous carbon fiber cloth (Ly-ACF-F40). By the technical route of thermal stabilization---sonication assisted phosphoric acid activation---hydrogen bonds introduced by interfacial fluorination, the constructed Ly-ACF-F40 acquires a high specific surface area (1870 m 2 /g) and total pore volume (1.277 cm 3 /g), and an excellent hydrogen storage capacity of 3.22 wt% under ambient pressure conditions (77 K, 1 bar). The study directly demonstrated in the experiment that dipole induced hydrogen bonding H(I)-H(II)···F can effectively enhance the atmospheric hydrogen storage density on the basis of other eliminating influencing factors of specific surface area. The simple construction strategy of porous carbon-based materials can provide reference for the research of unsaturated adsorption hydrogen storage materials under ambient pressure conditions, also assist in the application and promotion of low-cost solid hydrogen storage materials.
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Molecular Catalysis
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2024
·
IF 3.9
Yang Chen,Yatao Yan,Mengting Shao,Yongjian Xu,Guowang Diao,Ming Chen
In this work, N, P-Co 4 S 3 /NC nanospheres were successfully synthesized by double ligand strategy, followed by calcination and phosphating. By adjusting the radio of methimazole and 2-methylimidazole, and changing the calcination temperature, we obtained the optimal hydrogen evolution catalyst. The doping of N and P can regulate the electronic structure of Co, and further improve the electrocatalytic hydrogen production performance. Furthermore, N from dual ligands can form nitrogen-doped carbon, thus enhancing the conductivity and stability of the catalyst. The experimental results showed that N, P-Co 4 S 3 /NC exhibited good full pH activity in 0.5 M H 2 SO 4 , 1.0 M PBS and 1.0 M KOH, and the overpotentials of 163, 185 and 168 mV were required to reach the current density of 10 mA cm −2 , respectively. In this study, the dual ligands strategy can propose a new path for the design and synthesis of the catalyst precursor, and N, P codoping can effectively enhance the catalyst performance.
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Nanoscale
·
2012
·Vol. 4
·期 24
·7817-7824
·
IF 5.914
Yang Wang,Shouchuan Li,Hui Shi,Ke Yu
Two kinds of Cu2O–ZnO nano-heteroarchitectures were fabricated through a hydrothermal method. By utilizing polyethyleneimine (PEI) as a binding agent, ZnO nanoparticles were uniformly self-assembled onto Cu2O micro structures. Photoluminescence (PL), field emission and photocatalytic activities of the composite samples were investigated and compared with those of the pure Cu2O samples. The results reveal that ZnO nanoparticles combined on Cu2O microstructures remarkably changed the PL signals, and significantly enhanced the field emission and photocatalytic activities. The novel PL properties, enhanced field emission and photocatalysis activities are attributed to the electron transition and the inhibition of photo-induced electron–hole pairs recombination, which stem from interfacial defect states and energy band differentials at the interface of Cu2O and ZnO. The surface nano-protrusions, large surface area and better dye adsorption induced by ZnO nanoparticles are responsible for the field emission and photocatalysis improvements as well.
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JOURNAL OF FLUORESCENCE
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2024
·
IF 2.6
Li Qianwen,Yin Yu,Wang Wenjuan,Liu Bin,Tong Wei,Zhang Xu,Liu Jinquan,Yang Shengyuan
Herein, a visual and luminescent dual-mode (colorimetric and fluorometric) method for the detection of P-phenylenediamine (PPD) in hair dye was successfully established based on cerium-nitrogen co-doped carbon dots (Ce, N-CDs) that displayed remarkable luminescence and peroxidase activity. Ce, N-CDs catalyzed H 2 O 2 to produce superoxide anion, which then oxidized the colorless 3,3,5,5-tetramethylbenzidine (TMB) into blue oxidized TMB (oxTMB), capable of quenching the fluorescence through fluorescence resonance energy transfer (FRET) between Ce, N-CDs and oxTMB. The reducing properties of PPD could reduce oxTMB back to TMB, leading to a decrease in the absorption intensity of oxTMB and a fluorescence recovery of Ce, N-CDs. As a result, the quantitative detection of PPD could be achieved by measuring the absorption values of oxTMB and the fluorescence signal of Ce, N-CDs. The detection limits for PPD were calculated as 0.36 µM and 0.10 µM for colorimetry and fluorimetry, respectively. Furthermore, smartphone application (ColorPicker) capable of measuring the RGB value of the color was utilized in the detection system, facilitating on-site quantitative detection. This approach effectively shortens the detection time and simplifies the operation, offering a powerful and convenient tool for real-time monitoring of PPD.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xuan Zhou,Rongzhi Li,Fei Fu,Minggui Shen,Qiaoguang Li,He Liu,Xu Xu,Zhanqian Song
Most epoxy resins on the market have low thermal stability and flammable defects. As a potential curing agent for epoxy resin, polybenzoxazine (PBz) can effectively improve the thermal properties of the resin due to its low heat release capacity (HRC) and rigid aromatic ring support, and its raw materials can be derived from renewable resources. Here, we have successfully developed a molecular design strategy to obtain a trifunctional benzoxazine monomer with phosphate ester. Firstly, guaiacol-ethanolamine benzoxazine monomer (GE) was synthesized by Mannich condensation using guaiacol and ethanolamine as raw materials. Then trifunctional benzoxazine phosphate ester (TBP) was synthesized by the nucleophilic reaction of GE with phosphorus oxychloride. Finally, the epoxy resin DGEBA was cured by TBP to obtain a PBz modified epoxy resin (EP-TBP polymer) with T g of 113.7 °C and char yield of 37.4 %. Due to the introduction of TBP rich in phosphorus and nitrogen, it releases phosphorus radicals and nitrogen-containing inert gases during combustion, which leads to quenching effect and dilution effect. In addition, TBP can also promote the dehydration and dehydrogenation of the polymer and accelerate the formation of the aromatic hybrid char layer. Therefore, the THR of TBP modified epoxy resin is 49.3 % lower than that of epoxy resin without TBP, and the char yield is 47 times higher. And when the phosphorus content is 1.76 %, the flame-retardant grade can reach V-0. In addition, the introduction of TBP also enhanced the mechanical properties, adhesion properties and hydrophobicity properties of the polymer. It is worth mentioning that under alkaline conditions, the phosphate ester in the structure of EP-TBP polymer will undergo ammonolysis reaction with ethanolamine, and the resulting oligomers will be dissolved in it, thereby achieving rapid degradation of EP-TBP polymer. This work is to develop a high-performance multifunctional epoxy resin flame retardant curing agent based on renewable raw materials, and provide important insights for the subsequent development of halogen-free bio-based PBz flame retardant materials.
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