INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Qiang-Qiang Ma,Peng Zhou,Yizhen Liu,Zuowei Xie
Transition metal catalyzed selective cage B–H functionalization of carboranes has made significant progress in recent years, giving rise to the efficient synthesis of a large variety of cage B-functionalized carboranes including alkenylation, arylation, alkynylation, borylation, hydroxylation, acyloxylation, amination, and halogenation. However, the mechanisms of these catalytic B–X coupling reactions are not well understood. Herein, we describe the isolation and characterization of the catalytically relevant o-carborane based palladium(II) metallacycle, disclosing the details of Pd-catalyzed B–H functionalization of o-carboranes. As a result, highly selective catalytic B(3,6)-dihalogenation, -dimethylation, and -diarylation of o-carboranes have been achieved.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Tao Shan,Sunzai Ke,Xin Yang,Xuhui Yang,Bo Weng,Lijuan Shen,Min-Quan Yang
Photocatalytic selective oxidation of aromatic hydrocarbons plays an important role in the production of value-added chemicals. A key step in this process is the activation of C(sp 3 )-H bond by photogenerated holes. However, the inadequate hole generation and lack of surface adsorption-activation sites severely hinders the improvement in photocatalytic C-H bond oxidation. In particular, the random charge migration to the surface impedes the effective capture of holes by surface active sites to dissociate the C(sp 3 )-H bond. Here, we design and fabricate a Co 3 O 4 /Cs 3 Sb 2 Br 9 p-n heterojunction that effectively addresses these challenges. The p-n heterojunction forms strong built-in electric fields (BEF) facilitating spatial charge separation. Holes are accumulated on Co 3 O 4 , while electrons are accumulated on Cs 3 Sb 2 Br 9 , thereby offering abundant active holes and electrons. Moreover, Co 3 O 4 shows stronger adsorption and activation capacity for the C(sp³)-H bond, enabling the C(sp 3 )-H bond dissociation with low reaction energy barrier. Consequently, the holes are directionally extracted from photoactive Cs 3 Sb 2 Br 9 to catalytically active Co 3 O 4 under visible light irradiation, thereby accelerating the toluene oxidation. The optimized 5 % Co 3 O 4 /Cs 3 Sb 2 Br 9 exhibits a benzyl aldehyde (BAD) evolution rate of 5044 μmol g −1 h −1 and a benzyl alcohol (BA) production rate of 1820 μmol g −1 h −1 , which are 12 and 17 times higher than that of blank Cs 3 Sb 2 Br 9 , respectively.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinqi Luan,Xuehui Jia,Syed Jalil Shah,Jingyu Bao,Shunxiang Qin,Ruimeng Wang,Jiguang Deng,Zhongxing Zhao,Zhenxia Zhao
Low adsorption efficiency and secondary pollution release pose a bottleneck for the efficient capture of radioactive iodine vapor during nuclear utilization via adsorption. In addition, the simultaneous adsorption of iodine vapor alongside other harmful vapors in complex systems has been rarely reported. In this work, an electron/H-donating defective pore construction strategy involving MIL-101 modification via amino acids (AAs) was proposed to enhance its simultaneous adsorption efficiency for iodine and formaldehyde vapors. These defective microenvironments possessed microporous property with 11.3 Å, which not only formed strong affinity for I 2 molecules itself but also enhanced its adsorption interaction towards polyiodide anion (I 3 - and I 5 - ) through electron donation of AAs. Moreover, these adsorbed polyiodide anions and AAs-SL within the MOFs, resulting in multisite capture of FA via NH…O-H…I hydrogen bonding. The results revealed that AAs coordinated MIL-101 exhibited superior removal rate ( k 80% = 0.61–1.15 g g −1 h −1 ) for iodine vapor than that of the original MIL-101, which was 3.6–30.8 times higher that of state-of-the-art adsorbents under similar conditions. Notably, a high-capacity superior retention rate of 94.8 % was achieved for its I 2 adsorption after exposure to air for 7 days. After adsorption of iodine, AAs coordinated MIL-101 retained high FA adsorption capacity up to 9.7–12.9 mg/g, representing 75.1 %–87.7 % of the original AAs@MIL adsorption capacity for FA. This defective engineering strategy in MOFs supplied an efficient method for removing multiple harmful gases from the surrounding nuclear waste atmosphere.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Kuang Wang,Zhanqiang Fang
In the homologous series of polybrominated diphenyl ethers (PBDEs), the debromination of low-brominated diphenyl ethers with higher toxicity remains a challenge. Nano zero-valent iron (nZVI) has been extensively studied for the debromination of PBDEs, but its inherent direct electron transfer mechanism is less efficient for low-brominated diphenyl ethers, and there are issues with high preparation costs. In this work, we synthesize Ni-doped oxalated submicron ZVI (Fe OX bm /Ni) using a low-cost ball-milling method. Fe OX bm /Ni exhibits a debromination rate constant of 0.48 day −1 for 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in tetrahydrofuran (THF)/water. The debromination rate of Fe OX bm /Ni for BDE-47 in water is even faster (0.98 day −1 ), with the yield of the complete debromination product, diphenyl ether, reaching 76.71%. In real groundwater, Fe OX bm /Ni also shows high reactivity toward BDE-47, with a rate constant of 0.33 day −1 . Kinetic experiments, quenching experiments, and degradation pathway indicate that the attack of atomic hydrogen on C-Br bonds is the primary degradation mechanism. Electrochemical analysis further show that Ni 0 sites could cleave hydrogen into absorbed atomic hydrogen (H∗ ABS ) and adsorbed atomic hydrogen (H∗ ADS ), with H∗ ADS playing the main role. These findings contribute valuable insights into advancing the large-scale application of ZVI and offer promising strategies for thorough remediation of PBDEs pollution.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ji Shu,Yichong Zhang,Kanming Wang,Jianli Wang,Jiaxuan Ying,Hongyu Wang
Membrane filtration is regarded as one of the promising technologies for water treatment. However, insufficient micropollutants removal and membrane fouling still limited the further application. Herein, this study engineered a novel membrane hybrid system integrating typical pharmaceuticals removal and membrane self-cleaning by assembled layered MXene and hexagonal boron nitride (h-BN). By doping a small amount of MXene into h-BN (mass ratio of 1 to 10), the synergetic process of adsorption and photocatalytic degradation were achieved. Based on experimental and density functional theory (DFT) calculation results, the chemisorption-photodegradation performance of the membrane hybrid system assembled with 1/10 MXene@h-BN was significantly enhanced due to the termination group and conductive property of MXene. In addition, trimethoprim (TMP) degradation by the above membrane followed the Langmuir–Hinshelwood model, indicating pollutants removal initiated not only on the membrane surface but also in the bulk solution under simulated solar irradiation. This phenomenon was attributed to the generation of •OH and 1 O 2 by forming Ohmic contact with altered internal band structure. The durability and practical experiments with secondary effluent from local wastewater treatment were also tested. The exceptional self-cleaning performance of the membrane hybrid system assembled with 1/10 MXene@h-BN was demonstrated by lower membrane fouling and maintaining durability even after five cycles. Furthermore, the performance (both pollutants removal and flux) of the modified membrane for secondary effluent treatment was also considerable, validating its potential for practical application. Owing to the excellent features, the membrane assembled with MXene@h-BN is anticipated to be an ideal candidate for advanced wastewater treatment.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Yuhui Fu,Lijuan Dai,Sisi Wei,Yuxin Fang,Zhe Zhang,Hongtao Zhu,Tongwei Zhang,Lianmei Zhao,Baoen Shan
Esophageal squamous cell carcinoma (ESCC) represents a globally prevalent malignancy characterized by a poor prognosis, largely due to the challenges that patients face in tolerating invasive diagnostic procedures. Therefore, it is imperative to explore strategies to enhance the early diagnostic rate for patients with ESCC. Based on the property of H-chain ferritin-based magnetic ferritin nanoparticles (M-HFn) as contrast agents that can target cluster of differentiation 71 (CD71), this study provides a comprehensive evaluation of the expression levels and diagnostic potential of CD71 to investigate the feasibility of utilizing M-HFn for non-invasive diagnosis. Following the synthesis and the characterization of M-HFn, an orthotopic mouse model is developed to simulate the progression of ESCC. Subsequently, magnetic resonance imaging (MRI) scans are conducted after administering M-HFn to the mice. The results indicate a progressive increase of CD71 expression in tissues, transitioning from normal epithelium to esophageal squamous precancerous lesions (ESPL) and ultimately to ESCC. M-HFn injected into the mice selectively target cells with heightened CD71 expression, resulting in accumulation at the lesion sites. Consistent with pathological diagnoses, MRI images demonstrate a reduction in signal intensity at the lesion site in T 2 -weighted sequences, thereby facilitating the visualization of ESCC and ESPL. CD71 demonstrates high accuracy and specificity as a diagnostic target, positioning M-HFn-mediated targeted diagnostic strategy as a promising approach for the early detection of ESCC, with the potential to significantly improve patient prognosis.
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JOURNAL OF FOOD SCIENCE
·
2025
·Vol. 90
·期 8
·e70432
·
IF 3.4
Qin Geng,David Julian McClements,Taotao Dai,Wenlong Zhou,Zhihua Wu,Hongbing Chen
The molecular structure and surface properties of peanut proteins are altered by their non-covalent interactions with food polyphenols, which alter their allergenicity. In our research, the interactions between the critical peanut allergen (Ara h 2) and a model polyphenol (tannic acid [TA]) were studied utilizing experimental (spectroscopy and calorimetry) and molecular docking methods. Ultraviolet (UV) and circular dichroism (CD) spectroscopy analysis indicated that the microenvironment polarity and secondary/tertiary structure of Ara h 2 were changed due to its interaction with TA. Specifically, degree of molecular disorder increased, and the surface hydrophobicity of the polypeptide decreased after Ara h 2 interacted with TA. Analysis using fluorescence quenching, isothermal titration calorimetry, and molecular docking showed that the main non-covalent interactions were hydrogen bond formation between the Ara h 2 and TA. Binding site analysis using molecular docking indicated that the TA may have interacted with specific amino acids in the polypeptide chain, including Lys 31, Arg 34, Asp 35, Trp 44, Ser 54, Arg 59, Arg 60, Arg 122, Glu 123, and Gln 130. These amino acids are known to be part of the IgE epitope regions of Ara h 2, and so TA binding might be expected to impact peanut protein allergenicity. Indeed, an enzyme-linked immunosorbent assay (ELISA) study indicated that the IgE binding capacity of Ara h 2 was reduced after interacting with TA in a dose-dependent manner. This study enriches the understanding of the interactions between peanut protein allergens and small-molecule nutrients and provides a method for reducing the potential allergenicity of Ara h 2. Practical applications Employing the plant polyphenols as a means to modulate the activity of food allergens could potentially offer a breakthrough in managing food allergies. The strategic non-covalent binding of polyphenols, exemplified by TA, to the peanut allergen Ara h 2, may effectively lower its capacity to trigger allergic reactions, thereby offering an approach to mitigating peanut sensitization risks. The study examined the alterations in the structure and allergenic properties of Ara h 2 following its interaction with TA. This investigation was poised to accelerate the identification of TA's potential to inhibit peanut-induced allergic responses through allergen binding.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Huanji Song,Jiahao Sun,Lingshan Miao,Zhilong Lin,Shenghu Wang,Dongcheng Li,Weiyang Lv
Non-metallic catalysts have gained great attention in peroxymonosulfate based advanced oxidation processes (PMS-AOPs) for their enhanced safety and environmental compatibility. However, low catalytic efficiency, incomplete mineralization and harsh preparation methods still hinder their practical application. This work developed an innovative solvent-free ball milling-assisted pyrolysis strategy utilizing hexagonal boron nitride (h-BN) and multi-walled carbon nanotubes (MWCNTs) as synergistic precursors to construct the BN-CNT-700 composite. The mutually doped active sites were facilely formed through carbon/nitrogen hybridization , where electron-withdrawing C O groups dominated 1 O 2 generation while electron-donating C N sites primarily mediated SO 4 •− production. The radical and non-radical pathways worked in synergy to achieve complete removal of 20 mg·L −1 bisphenol A (BPA) coupled with an ultra-high mineralization efficiency of 88.6 %, surpassing most reported non-metallic counterparts and even outperforming various metal-based systems. Moreover, the BN-CNT-700/PMS system demonstrated exceptional environmental robustness, maintaining high BPA removal efficiency across broad pH ranges, various inorganic ions, and complex water matrices. This research offers the important implications for the rational design of non-metallic catalysts with tunable active sites for high-efficiency pollutant decontamination.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ping Ye,Weimiao Wang,Xiaodong Li,Zhiqiang Qiao,Yirui Lu,Bing Huang,Liangfei Bai,Liang Chen,Xiaoqing Tu,Rui Li,Guangcheng Yang,Guoqing Lv
Although laser ignition is considered to be one of the most promising ways to detonate energetic materials due to its high safety and reliability, it is still a challenge to achieve direct ignition of energetic materials by a laser with low-power and near-infrared (NIR) band. In this paper, a molecular self-assembly strategy based on recrystallization was utilized to prepare 4,4′,5,5′-tetranitro-1H,1′H-[2,2′-biimidazole]-1,1′-diamine (DATNBI) crystals with various micro-nano structures. The characterization results suggest that DATNBI crystals with different degrees of roughness and defects by the induction of solvents and surfactants. The crystal defects can not only bring about the enhancement of light absorption of DATNBI in NIR band, but also advance its thermal decomposition, providing reliable support for direct laser ignition of DATNBI profit from the hot spot ignition theory. Combined with density functional theory, it is speculated that electrons of defect states achieve electron-hole recombination by laser radiation, thereby enhancing photothermal conversion. Compared with raw DATNBI, DATNBI crystals with rough surface and abundant defects can be directly ignited by a NIR laser and exhibits self-sustainable combustion. In summary, a direct NIR laser-ignitable energetic material has been prepared via appropriate crystal structure design.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2024
·
IF 4.1
Luo Fang-Hua,Dong Zhi-Tao,Chen Guo-Hua,Ma Chen,Wang Huai-Yuan
Janus films with asymmetric physical/chemical properties have attracted considerable attention due to their promising applications in personal thermal management, electronic skins, sensors, actuators, etc. However, traditional methods for fabricating Janus films conventionally need the assistance of an interface or auxiliary equipment, which are usually complex and time-consuming. Herein, flexible poly(vinyl alcohol) (PVA)/graphene oxide (GO)/h-BN (recorded as PVA/GO/h-BN) Janus films with thermally, optically, and electrically anisotropic properties are fabricated by a simple density deposition self-assembly method, which just utilizes the density difference between GO and h-BN during water evaporation. Experimental results show that the two sides of the acquired Janus films have obvious asymmetric characteristics. In the original state of the PVA/GO/h-BN Janus films, the thermal conductivity of the GO side (10.06 W·m −1 ·K −1 ) is generally lower than that of the h-BN side (10.48 W·m −1 ·K −1 ). But after GO is reduced, the thermal conductivity of the rGO side reaches 12.17 W·m −1 ·K −1 , surpassing that of the h-BN side. In addition, the relative reflectance of the h-BN side of Janus film is also significantly higher than that of the rGO side, and the surface resistance difference between the two sides is about 4 orders of magnitude. The prepared PVA/GO/h-BN Janus films show great application potential in human thermal management, light conversion switches, and electronic skins. This study provides a simple and versatile strategy for fabricating Janus films with multifunctional (such as thermal, optical, and electrical) anisotropies.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ge Shu,Yuda Li,Zhuang Wang,Jia-Xing Jiang,Feng Wang
Conjugated polymers have recently emerged as encouraging metal-free photocatalysts for solar energy conversion under visible light irradiation. Unfortunately, photocatalytic activities of the current polymers are still inadequate. Herein, we present a simple but quite attractive conjugated homopolymer (PDBTSO) based a dibenzothiophene-S,S-dioxide moiety. The introduction of sulphonyl group to a polyfluorene-like backbone can cause richly available active sites and lead to the efficient separation of photoexcited charge carriers, thus yielding impressive photocatalytic performance. Furthermore, we explored a natural “phosphorylation” strategy for increasing photocatalytic hydrogen production over PDBTSO. Remarkably, an extremely high hydrogen evolution rate of 44.2 mmol h −1 g −1 was achieved with the optimum addition of K 2 HPO 4 under visible light irradiation.
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POLYMER SCIENCE SERIES B
·
2015
·Vol. 57
·期 5
·460-472
·
IF 0.577
Sa Zongpeng,Li Yapeng,Zhao Haochen,Hu Qi,Wei Jia,Wang Jingyuan
Through H-shaped macroinitiator glycol-chlorine((Cl) 2 -PEG-(Cl) 2 ) to initiate the ATRP reaction of 2-Hydroxyethyl Methacrylate (HEMA) we synthesized H-shaped copolymer (PHEMA) 2 - b -PEG- b -(PHEMA) 2 . After we modified the copolymer with histidine (His), the self-assembling and drug release behavior was studied. The morphology of the copolymer micelles and drug loaded micelles were examined by transmission electron microscope (TEM). Spherical micelles and core-shell structure with a diameter of 165 nm were obtained (at pH = 7.0). Due to the presence of imidazole-ring in histidine the copolymer show commendable pH-sensitivity, which made the copolymer potential application as drug carrier exhibiting good control-released property.
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