Acta Biomaterialia
·
2023
·
IF 9.7
Chun-chi Lei,Jie Lei,Xiao-guang Zhang,Hong-chuan Wang,Ya-qi He,Wei-feng Zhang,Bi-de Tong,Cao Yang,Xiao-bo Feng
Infection of bone defects remains a challenging issue in clinical practice, resulting in various complications. The current clinical treatments include antibiotic therapy and surgical debridement, which can cause drug-resistance and potential postoperative complications. Therefore, there is an urgent need for an efficient treatment to sterilize and promote bone repair in situ . In this work, an ultrasound responsive selenium modified barium titanate nanoparticle (Se@BTO NP) was fabricated, which exhibited significant antibacterial and bone regeneration effects. Selenium nanoparticle (Se NP) was modified on the surface of barium titanate nanoparticle (BTO NP) to form heterostructure, which facilitated the second distribution of piezo-induced carriers under ultrasound (US) irradiation and improved the separation of electron-hole pairs. The Se@BTO NPs exhibited remarkable antibacterial efficiency with an antibacterial rate of 99.23% against Staphylococcus aureus ( S.aureus ) and significantly promoted the osteogenic differentiation under ultrasound irradiation. The in vivo experiments exhibited that Se@BTO NPs successfully repaired the femoral condylar bone defects of rats infected by S.aureus , resulting in significant promotion of bone regeneration. Overall, this work provided an innovative strategy for the utilization of US responsive nanomaterials in efficient bacteria elimination and bone regeneration. Statement of Significance Infectious bone defects remain a challenging issue in clinical practice. Current antibiotic therapy and surgical debridement has numerous limitations such as drug-resistance and potential complications. Herein, we designed an innovative ultrasound responsive selenium modified barium titanate nanoparticle (Se@BTO NP) to achieve efficient non-invasive bacteria elimination and bone regeneration. In this work, Se@BTO nanoparticles can enhance the separation of electrons and holes, facilitate the transfer of free carriers due to the cooperative effect of ultrasound induced piezoelectric field and heterojunction construction, and thus exhibit remarkable antibacterial and osteogenesis effect. Overall, our study provided a promising strategy for the utilization of piezocatalytic nanomaterials in efficient antibacterial and bone regeneration.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Man Yang,Zhenzhen Shi,Shaodong Sun,Bian Yang,Jie Cui,Jianing Li,Daqin Yun,Nian Lei
Developing heterojunction photocatalyst with well-matched interfaces and multiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal, but still remains a great challenge. In present work, a new strategy of chloride anion intercalation in Bi 2 O 3 via one-pot hydrothermal process is proposed. The as-prepared Ta-BiOCl/Bi 24 O 31 Cl 10 (TBB) heterojunctions are featured with Ta-Bi 24 O 31 Cl 10 and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces. In this TBB heterojunctions, the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer and multiple transfer paths, respectively, leading to enhanced visible light response and improved photogenerated charge separation. Meanwhile, a type-II heterojunction for photocharge separation has been obtained, in which photogenerated electrons are drove from the CB (conduction band) of Ta-Bi 24 O 31 Cl 10 to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl, while the photogenerated holes are left on the VB (valence band) of Ta-Bi 24 O 31 Cl 10 , effectively hindering the recombination of photogenerated electron-hole pairs. Furthermore, the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species (·O 2 − ). Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride (TCH) solution to Bi 2 O 3 , Ta-BiOCl and Ta-Bi 24 O 31 Cl 10 . This work not only proposes a Ta-BiOCl/Bi 24 O 31 Cl 10 shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-II heterojunction for highly efficient photocatalytic activity, but offers a new insight into the design of highly efficient heterojunction through phase-structure synergistic transformation strategy.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Caiwen Wu,Tianyi Guo,Yuhan Chen,Qiang Tian,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Photoinduction is widely used to accelerate the Fe 3+ /Fe 2+ circulation in Fe 3+ /H 2 O 2 Fenton oxidation, however, the remained challenges in developing a facile, economical, and efficient synthetic methodology for the preparation of high-performance Fe-based Photo-Fenton catalyst and inevitably forming iron sludge limit its applications. Herein, starch-derived carbon (SC) encapsulated Fe 3 O 4 (Fe 3 O 4 @SC) magnetic nanocomposites are synthesized by mechanical activation treatment combined with high-temperature pyrolysis method using cassava starch as the carbon source. The photoelectrochemical properties of Fe 3 O 4 @SC are regulated by C O Fe bonds and oxygen vacancies in Fe 3 O 4 @SC, as well as graphitization of SC, which effectively accelerate the Fe 3+ /Fe 2+ circulation in Fe 3 O 4 @SC + H 2 O 2 system under visible light, thus Fe 3 O 4 @SC shows excellent catalytic performance and superior stability for the degradation of tetracycline hydrochloride, and the initiation rate constant is 2.4 times higher than that in dark. Moreover, quenching experiments and electron spin resonance results confirm that OH, O 2 − , and h + ( OH plays a critical role) are generated in the catalytic system of Fe 3 O 4 @SC + H 2 O 2 + visible light. This work provides new insights into a green and facile approach for the synthesis of Photo-Fenton catalysts, providing new avenue for the acceleration of Fe 3+ /Fe 2+ cycle under visible light-driven Fenton process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Haoyue Li,Na Wang,Han Li,Ziqiu Ren,Wenjie Ma,Jun Li,Yunchen Du,Qun Xu
Fe-based N-doped carbon catalysts (Fe/NC-XPVP) are synthesized through a solvent-free and one-step pyrolysis strategy, allowing for the control of Fe active center sizes and the morphology of carbon substrates. The variable-sized Fe active centers in Fe/NC-XPVP exhibit size-dependent catalytic behavior in peroxymonosulfate (PMS) activation reaction, which indicates that downsizing Fe particles to atomic level achieves performance improvement and mechanism transformation from radical to non-radical pathway. The optimal Fe/NC-1.0PVP catalyst can realize nearly 100.0 % of tetracycline degradation efficiency within 30 min. Density functional theory calculations demonstrate that the strong adsorption of PMS onto Fe-N 4 sites can promote the formation of catalyst/PMS* complexes and induce the occurrence of electron transfer process, which performs great resistance to complex water environments during PMS activation. This work gives valuable insights into the precise design and regulation of metal active sites on N-doped carbon materials and provides a promising catalyst for wastewater remediation.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Ying Mei,Yushan Huang,Haochen Xu,Wulin Yang,Xiaocheng Lin
Fouling control is the most critical concern in the implementation of nanofiltration (NF) for dye wastewater treatment . In this study, integration of NF and Fenton-like advanced oxidation was realized by tailoring a thin film composite NF membrane (TFNi) with in situ synthesized PDA/MnO 2 interlayer. TFNi was optimized by controlling the amount of MnO 2 nanoparticles incorporated within the interlayer which endowed the membrane with self-cleaning property. Besides it improved the membrane surface hydrophilicity and optimized the water transport path, resulting in alleviated fouling risks and an enhanced water permeance of 24 ± 2 L m −2 h −1 bar −1 compared to the control membrane. Fouling and subsequent chemical cleaning experiments were carried out on TFNi under various water chemistry conditions to elucidate the underlying mechanisms governing the self-cleaning properties. Accordingly, a high flux recovery ratio ( FRR ) (above 95%) was maintained thanks to the generation of free radicals by MnO 2 –H 2 O 2 system which was validated by determining the free radical scavenging activities. Moreover, the interlayer confined radicals can facilitate the decomposition of foulants on TFNi. Conclusively, H 2 O 2 -initiated self-cleaning of TFNi can be of great prospect for the efficient treatment of dye wastewater via in-situ generated free radicals.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Junyong He,Ya Yang,Peidong Hong,Yulian Li,Chao Xie,Zijian Wu,Minqiang Li,Lingtao Kong
The use of peroxymonosulfate (PMS) activation to eliminate organic contaminants is a promising technology to purify water owing to its strong reactivity. However, because of the existed rate limiting step, the performance of PMS activation was restrained and required external energy consumption. Therefore, a new strategy was proposed to solve this problem by preparing catalysts with abundant electron-rich sites and electron traps to accelerate PMS activation. In this research, a novel MnCeO x -H catalyst with rich surface oxygen vacancies was firstly synthesized to accelerate the transfer of electrons among the catalysts, oxidant and pollutants. The contaminants were rapidly eliminated in the MnCeO x -H/PMS system, while the reaction rate constant of MnCeO x -H/PMS system was 30 times higher than that of CeO 2 /PMS system. The surface oxygen vacancies were able to adsorb and trap PMS, then the free electrons of oxygen vacancies would reduce PMS and produced HO•, 1 O 2 and SO 4 •- , while 1 O 2 played a major role. The contaminants which acted as electron-donors in this system were adsorbed at Mn, Ce sites, achieving effective conversion recycling of Ce(IV)/Ce(III), Mn(III)/Mn(II) and Mn(IV)/Mn(III). This discovery is believed to inaugurate a novel way for designing powerful electron-rich sites and electron traps to accelerate PMS activation for contaminants degradation.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Meijuan Lan,Tongshuai Li,Lin Li,Shaoyun Wang,Juncheng Chen,Tangyu Yang,Zhiru Li,Yipeng Yang,Xia Zhang,Bing Li
The physiochemical properties, structure characteristics, oxidation, and emulsifying properties of myofibrillar proteins (MPs) in low salt solution after treated by the ultrasound were investigated. The solubility, mean diameters, sulfhydryl content, and carbonyl contents of MPs after ultrasonic treatment increased, while the turbidity decreased. The surface hydrophobicity of MPs with 200 W–600 W treatment increased, but decreased at 800 W treatment. The circular dichroism analysis revealed that α-helix content increased, while β-sheet and random coil content decreased after ultrasonic treatment. Fluorescence spectroscopy indicated the fluorescence intensities of MPs were increased after ultrasonic treatment. SDS-PAGE results showed more protein polymers due to myosin heavy chain (MHC) aggregation via disulfide bonds. Based on LC-MS/MS result, the myosin heavy chain was susceptible to oxidation, with monooxidation being the main oxidative modification. Finally, the emulsions stabilized by ultrasonically treated MPs, especially those treated at 800 W, exhibited decreased particle size, improved uniformity, and enhanced stability.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Nian Liu,Yuqi Zhang,Jiaoyan Huang,Sicong Liu,Taiping Qing,Peng Zhang,Bo Feng
In the realm of sensing, carbon dots (CDs) have exhibited remarkable fluorescence characteristics. In the field of catalysis, CDs can function concurrently as electron donors and acceptors and have substantial electron or hole transport capacities. In this study, both merits were integrated into one, and a one-step hydrothermal approach was used to create multifunctional CDs. On the one hand, CDs are employed as a fluorescence probe with good sensitivity and selectivity to detect Cr(VI). On the other hand, CDs exhibit strong photoreduction capabilities for Cr(VI) in the absence of any external cocatalysts or photosensitizers when acting as photoinitiators. The results show that Cr(VI) quenches the CDs fluorescence as a result of the combined effects of static quenching and the inner filter effect. At the same time, under the condition of illumination, the inner filter effect encourages the CDs electrons to move from the valence band to the conduction band, resulting in electron hole pairs. With the help of electrons' reducing power, Cr(VI) can be rapidly and effectively converted to Cr(III). The findings of this study suggest that CDs are a satisfying bi-functional carbon-based material with significant potential for the treatment of industrial wastewater.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Yougan Xiao,Jiahui Lu,Shunjian Cheng,Zilong Wang,Antong Shi,Jyunhong Shen,Zhuwu Jiang
From a preliminary performance comparison of several layered double hydroxides (LDHs), magnetically separable Ni-M LDHs (M = Fe, Al) were synthesized and applied as efficient ozonation catalysts for degrading dye Rhodamine B (RhB). As proved by various characterizations, the micromorphology, nanostructure size, and porous feature of the synthesized Ni-M LDHs significantly varied with different metal components. Among them, Ni 3 -Fe LDH and Ni 2 -Al LDH possessed a relatively larger specific surface area to react with O 3 interfacially, thereby exhibiting excellent catalytic ozonation performance. The RhB was almost completely degraded within 60 min, and the removal efficiencies of COD and TOC reached above 70% and 50%, respectively. The effects of catalyst dosage, initial dye concentration, solution pH, and coexisting inorganic anions on RhB degradation were studied systematically. ESR measurements and radical quenching experiments indicated that OH , O 2 − , and 1 O 2 are primary reactive oxygen species (ROS), while 1 O 2 induced the most dominant degradation contribution. According to the variations of ROS formation and material properties during the catalytic ozonation process, the possible reaction mechanisms were proposed. Moreover, the differences involved in the redox of multivalent metals and the transformation of surface hydroxyls over Ni-Fe and Ni-Al LDHs were further revealed.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 11
·4441-4447
·
IF 1.6
Zhou Dan,Guo Yadan,Wang Juan,Xuan Keng,Guo Yaoping,Jiang Hao,Wang Xuegang,Zhou Zhongkui
This study investigated the use of ultraviolet (UV) light irradiation for the activation of formic acid (FA) to reduce U(VI) in aqueous solutions. The results demonstrated that under UV radiation, FA exhibited a higher U(VI) reduction efficiency than other organic acids, and up to 70% of U(VI) in aqueous solutions was successfully removed. Electron spin resonance and methanol quenching experiments confirmed that U(VI) reduction in the UV/FA process was due to the electron transfer facilitated by FA (HCOOH) and CO 2 •− . This catalyst-free UV/FA process holds promise for the reduction of U(VI) in leaking water from uranium tailing ponds.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 39
·e2305883120
·
IF 11.1
Chencheng Dong,Zhi-qiang Wang,Chao Yang,Xiaomeng Hu,Pei Wang,Xue-qing Gong,Lin Lin,Xiao-yan Li
Inspired by the development of single-atom catalysts (SACs), the fabrication of multimetallic SACs can be a promising technical approach for the in situ electro-Fenton (EF) process. Herein, dual-functional atomically dispersed Mo–Fe sites embedded in carbon nitride (C3N5) (i.e., MoFe/C3N5) were synthesized via a facile SiO2 template method. The atomically isolated bimetallic configuration in MoFe/C3N5 was identified by combining the microscopic and spectroscopic techniques. The MoFe/C3N5 catalyst on the cathode exhibited a remarkable catalytic activity toward the three electron-dominated oxygen reduction reaction in sodium sulfate, leading to a highly effective EF reaction with a low overpotential for the removal of organic contaminants from wastewater. The new catalyst showed a superior performance over its conventional counterparts, owing to the dual functions of the dual-metal active sites. Density functional theory (DFT) analysis revealed that the dual-functional 50-MoFe/C3N5 catalyst enabled a synergistic action of the Mo–Fe dual single atomic centers, which can alter the adsorption/dissociation behavior and decrease the overall reaction barriers for effective organic oxidation during the EF process. This study not only sheds light on the controlled synthesis of atomically isolated catalyst materials but also provides deeper understanding of the structure–performance relationship of the nanocatalysts with dual active sites for the catalytic EF process. Additionally, the findings will promote the advanced catalysis for the treatment of emerging organic contaminants in water and wastewater.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Xiao-Juan Li,Ming-Yu Qi,Jing-Yu Li,Chang-Long Tan,Zi-Rong Tang,Yi-Jun Xu
The simultaneous utilization of photogenerated electrons and holes in one cooperative photoredox system for the dehydrocoupling of thiols into value-added disulfides and clean hydrogen (H 2 ) fuel meets the development criteria of green chemistry. Herein, we report the synthesis and application of cocatalyst PdS decorated ZnIn 2 S 4 (PdS-ZIS) composites for photocatalytic coupling of thiols into disulfides and H 2 evolution under visible light irradiation. The superior photocatalytic performance over PdS-ZIS composites compared with blank ZIS is attributed to the function of PdS as oxidation cocatalyst, which dramatically promotes the separation and transfer of photogenerated charge carriers due to its excellent hole trapping ability. In-situ Fourier transform infrared spectra reveal the dynamic variation of reactants on the catalyst surface. Electron paramagnetic resonance technology confirms that sulfur-centered radicals are the key reaction intermediates in this coupling process. Moreover, the application of PdS-ZIS composites to the dehydrocoupling of various thiols with different substituent groups into the corresponding S–S coupling products has been demonstrated to be practicable. This work is expected to offer insights into the rational design of cocatalyst-decorated semiconductor photocatalysts with efficient utilization of photogenerated electrons and holes for the co-production of high-value chemicals and clean H 2 energy in a cooperative photoredox catalysis process.
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