Journal of Cleaner Production
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2024
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IF 9.7
Zhengshuai Sun,Rujiao Jiang,Wenbin Hua,Qi Wei,Qiaoxia Yuan,Baojun Yi
Biomass-based graphitic carbon is a promising material, but the effect mechanism of inherent alkali metals on the catalytic pyrolysis of biomass is still unclear. In this study, cellulose was selected as the model substance, and the influence mechanism of Na on the graphitization of cellulose catalytic pyrolysis was investigated through a combination of experiments and theoretical calculations. The results indicate that Na can interact with the carbon skeleton through van der Waals forces, thereby altering the spatial structure of graphite crystals and increasing the interlayer spacing of graphite by 27.7%. In addition, Na can coexist with Fe(III) in the form of oxides, while also increasing the reaction energy barrier of reverse hydroxylation and dehydration cyclization, decreasing the generation of reducing gases mainly composed of CO. This impedes the reduction of iron-based catalysts, thereby affecting the formation of the graphite microcrystalline structure. The research indicates that maintaining the ratio of Na content to iron-based catalysts within a 1:1 range is optimal for producing graphite carbon from cellulose.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Changrong Zhao,Bin Liu,Tingting Zhu,Xuewu Zhu,Xiaoxiang Cheng
Advanced oxidation is an effective method for removing hard-to-degrade organic pollutants from water. In this paper, a novel structure of a single atom Fe anchored g-C 3 N 4 (FeCN) membrane was proposed to remove pollutants from water by coupling membrane technology with photocatalytic and peroxyacetic acid oxidation. The presence of zero-dimensional Fe atoms in FeCN membranes allows for the removal of acetaminophen (APAP) in mobile membrane filtration systems without compromising permeation performance by simultaneously possessing visible photocatalytic capability and peroxyacetic acid (PAA) activation. Existence of inter-membrane domain-limiting conditions led to 100 % degradation of APAP within 10.5 ms, which is 5 orders of magnitude faster than conventional catalytic systems. Notably, photo-generated electrons/holes generated by light and HClO generated by Cl - promote the conversion of Fe(V) and the removal of pollutants during the catalytic process. The spatial separation ability of the membrane catalytic layer surface mitigates the catalyst's passivation by macromolecular organics. Furthermore, surface photocatalysis of the membrane and interlayer catalysis generated by PAA mitigate the surface and interlayer pollutants of the membrane, respectively. This study explores a novel approach for the development of highly efficient atom-catalyzed membrane systems with multiple purposes.
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FOOD CHEMISTRY
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2023
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IF 8.8
Xinrou Wang,Huan Liu,Cailin Qiao,Yi Ma,Huibo Luo,Changjun Hou,Danqun Huo
Traditional methods of tannins detection suffer from complex pretreatment, long detection time, and limited sensitivity. Modern techniques like liquid chromatography require expertise, involve tedious result processing, and lack effective data visualization. Therefore, there is a need for an alternative detection method that simplifies pretreatment and detection steps, reduces analysis time, and provides visualized results. In this study, a novel colorimetric sensor based on single-atom Fe nanozyme (Fe@CN-20) was developed for tannins detection. Fe@CN-20 exhibited laccase-like and oxidase-like activities, enabling simultaneous oxidation of tannins and a substrate called TMB. Tannins competed with TMB, allowing quantification of tannins content. The Fe@CN-20/TMB system provided a detection range of 5–100 mg/L tannic acid, with a detection limit of 0.13 mg/L (S/N = 3). Analysis time was approximately 30 min. The platform successfully quantified tannins in brandy, showing less than 5% deviation compared to the standard method. The sensor was simple, sensitive, rapid, and provided strong visualization.
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Theranostics
·
2023
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IF 12.4
Wenjie Feng,Wanrui Shi,Yanqi Cui,Jiajun Xu,Shuwei Liu,Hang Gao,Shoujun Zhu,Yi Liu,Hao Zhang
Immunoadjuvants, as an indispensable component of tumor vaccines, can observably enhance the magnitude, breadth, and durability of antitumor immunity. However, current immunoadjuvants suffer from different issues such as weak immunogenicity, inadequate cellular internalization, poor circulation time, and mono-functional bioactivity. Methods: Herein, we construct Fe 3+ -Shikonin metal-phenolic networks (FeShik) nanomedicines as immunogenic cell death (ICD) stimulants and multifunctional immunoadjuvants for tumor vaccination. The multifunctionality of FeShik nanomedicines is investigated by loading ovalbumin (OVA) as the model antigen to construct OVA@FeShik nanovaccines or 4T1 tumor cell fragment (TF) as homologous antigen to construct TF@FeShik nanovaccines. In vitro examinations including GSH responsive, •OH generation, colloid stability, cellular uptake, cytotoxicity mechanism of ferroptosis and necroptosis, ICD effect, the promotion of DC maturation and antigen cross-presentation were studied. In vivo observations including pharmacokinetics and biodistribution, antitumor effect, abscopal effect, immune memory effect, and biosafety were performed. Results: The presence of FeShik nanomedicines can significantly prolong the blood circulation time of antigens, increasing the bioavailability of antigens. Upon phagocytosis by tumor cells, FeShik nanomedicines can disassemble into Fe 2+ and Shikonin in response to tumor microenvironments, leading to ICD of tumor cells via ferroptosis and necroptosis. Consequently, ICD-released autologous tumor cell lysates and pro-inflammatory cytokines not only stimulate DC maturation and antigen cross-presentation, but also promote macrophage repolarization and cytotoxic T lymphocyte infiltration, resulting in the activation of adaptive immune responses toward solid tumors. Conclusion: In a word, our FeShik supramolecular nanomedicines integrate bioactivities of ICD stimulants and immunoadjuvants, such as eradicating tumor cells, activating antitumor immune responses, modulating immunosuppressive tumor microenvironments, and biodegradation after immunotherapy. Encouraged by the diversity of polyphenols and metal ions, our research may provide a valuable paradigm to establish a large library for tumor vaccination.
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RARE METALS
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2020
·Vol. 40
·期 7
·1957-1965
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IF 2.161
Xu Yin-Long,Mo Rui-Xue,Qi Cai-Yu,Ren Zeng,Jia Xiu-Zhi,Kan Zi-Gui,Li Cao-Long,Wang Fei
Abstract The excitation wavelength-dependent and -independent emissions are two crucial fluorescent properties of carbon dots (CDs). However, CDs reported till date exhibit only one of these properties, which limits their practical applications. Herein, dual-property carbon dots (DCDs) with both the excitation wavelength-dependent and -independent emissions were synthesized via a facile one-step solvothermal method using 4-(2-pyridylazo)-resorcinol as the carbon precursor. The multi-functional applications of the resulting DCDs were also evaluated. The as-prepared DCDs exhibited not only excellent monodispersity, high photostability, and storage stability, but also low toxicity, good biocompatibility, and cellular bioimaging capability. In addition, the DCDs exhibited excitation-dependent emission photoluminescence under low excitation wavelengths. The DCDs exhibited good Fe 3+ detection by quenching the blue emission fluorescence and showed a relatively low Fe 3+ detection limit of 0.067 μmol·L −1 based on three times signal-to-noise criteria ( R 2 = 0.99). Furthermore, the DCDs showed excitation-independent emission at low excitation wavelengths and exhibited red emission at about 598 nm to avoid damage to the body. These results demonstrate the excellent bioimaging properties of the DCDs. Owing to their dual PL properties, the as-prepared DCDs exhibited multi-functional applications: Fe 3+ detection and A549 cell bioimaging. These results will be helpful in developing novel CDs for applications in various fields. Graphic abstract
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CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Yunjiang Yu,Zheng Huang,Dongyang Deng,Yongming Ju,Luyao Ren,Mingdeng Xiang,Liangzhong Li,Hui Li
Tetrabromobisphenol A (TBBPA) was a potential persistent organic pollutants. This study synthesized s-Fe/Cu bimetallic particles by decorated sponge iron (s-Fe) with Copper (Cu) to degrade TBBPA. S-Fe/Cu bimetallic particles was further characterized by XRD, XPS, SEM and EDS. The optimal TBBPA removal efficiency was 95.9%. Among the theoretical Cu mass loading increasing from 0 wt% to 6 wt%, 4 wt% mass loading was the best; with TBBPA initial concentration increased from 5 mg/L to 30 mg/L, TBBPA removal efficiency decreased from 91.2% to 73.0%; also, when dosage increased from 10 g/L to 30 g/L, removal efficiency increased from 58.1% to 95.9%; pH 6.5 were beneficial to degrading TBBPA and the s-Fe/Cu bimetallic particles showed strong catalytic ability after 4 reuse cycle. Kinetic analysis showed that the degradation of TBBPA obeyed pseudo-first-order kinetics. In addition, Liquid Chromatography Time-of-Flight Mass Spectrometry (LC/TOF/MS) detected degradation products including debromination products, hydroxylation products, single aromatic ring products and O -methylating product, which demonstrated that the main degradation pathway were debromination, hydroxyl, β -scission and O -methylation reactions.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wenlan Ji,Weiwei Li,Yuan Wang,Tian C. Zhang,Shaojun Yuan
The urgent need to remove arsenic from groundwater stems from the irreversible damage it causes to aquatic systems and biological health. In this study, unique magnetic Fe 3 O 4 /graphene oxide (GO) nanocomposites derived from MIL-100(Fe)/GO precursor were rationally and precisely developed by combination of solvothermal synthesis and pyrolysis methods. The optimized MIL-100(Fe)/1%GO-400 magnetic nanocomposite (where 1% and 400 represent the mass ratio of GO to MIL-100(Fe) and pyrolysis temperature, respectively) exhibited exceptional adsorption capacity for As(V) and possessed magnetic separation properties. The novel nanocomposite had complete MOF morphology and crystal structure, as well as good resistance to interference from ions and could be used effectively over a wide pH range (2–9) for adsorption of As(V). The As(V) adsorption on the nanocomposite was found to follow the pseudo-second-order (PSO) kinetic model and Temkin adsorption isotherm model, as well as a spontaneous endothermic process dominated by chemisorption. The incorporation of GO and pyrolysis of the Fe-MOFs was proven to enhance the adsorption capacity of nanocomposite, water stability, and magnetic recovery ability. The adsorption mechanism was attributed to the synergistic effect of chemical complexation, hydrogen binding and electrostatic interaction. This work not only presents a feasible strategy for the development of Fe-MOFs-based derivatives, but also offers a promising approach to expanding the application of functional Fe-MOFs-based derivatives in arsenic-contaminated wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yufeng Wang,Qing Ye,Lu Lin,Yanxia Zhao,Yongliang Cheng
Designing and fabricating highly competent and inexpensive electrocatalysts are highly desirable for application in electrocatalytic water splitting. In this study, we synthesized NiFeRu/C nanofibers and Ru, Fe dual-doped Ni 5 P 4 (Ru, Fe-Ni 5 P 4 )/C nanofibers as complementary electrocatalysts for overall water splitting through electrospinning, carbonization, and phosphorization treatment, respectively. The NiFeRu/C nanofibers and Ru, Fe-Ni 5 P 4 /C nanofibers showed high hydrogen evolution reaction and oxygen evolution reaction activity, respectively, due to the presence of numerous exposed active sites and optimized adsorption capacity for the reaction intermediates contributed by the synergistic interaction among different metal components in the electrocatalysts. Hence, the assembled asymmetrical electrolytic cell effectively promoted overall water splitting, requiring a voltage of 1.569, 1.744, and 1.872 V to achieve a current density of 100, 500, and 1,000 mA cm −2 , respectively, and it was better than Pt/C||IrO 2 . Additionally, the electrolytic cell could work at 500 mA cm −2 for 100 h without any noticeable deterioration in activity, which indicated that it was durable at high current density. In this study, we described a novel method for designing highly efficient electrocatalysts for overall water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shihui Zhang,Chang-an Zhou,Shenghong Wang,Zhifeng Qin,Guoqiang Shu,Chao Wang,Lei Song,Lirong Zheng,Xiaoyang Wei,Kui Ma,Hairong Yue
Selective oxidative dehydrogenation of propane with CO 2 (CO 2 -ODP) represents a promising pathway of propylene production and CO 2 utilization. Presently, vanadium (V) based catalysts are commonly used due to the excellent redox ability originated from the multivalent V. However, the CO 2 -ODP reaction mechanism remains elusive, limiting the rational design of highly efficient catalytic systems. Herein, we introduced Fe into impregnated V-Al 2 O 3 to build a dual-sites catalyst including Fe and V, achieving a C 3 H 8 conversion at ∼43 % and C 3 H 6 selectivity exceed 80 %. Via regulating the Fe/V molar ratio, we clearly describe that the formation of unique Fe-O-V facilitated the CO 2 dissociation. Intrinsically, V is the main active site contributing for C 3 H 8 dehydrogenation while Fe site is responsible for the CO 2 dissociation, replenishing lattice oxygen to enhance oxidative dehydrogenation of C 3 H 8 . The design of dual-sites catalyst and extraction of molecular understanding provide guidance for the rational development of highly active CO 2 -ODP catalysts.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Yuhang Li,Rui Cai,Kang Chen,Yujing Zhang,Xu Chen,Bo Sun,Yu Jiang,Chaochao Tan,Chuang Peng,Yinghui Song,Ling Wu,Sulai Liu
Severe acute pancreatitis (SAP) is a serious inflammatory disease that is often associated with high mortality rate. It tends to trigger a cascade of systemic inflammation that causes damage to multiple organs, such as the lungs and kidneys. Currently, there is no effective treatment plan to reverse the progress of SAP. The occurrence and development of SAP are associated with oxidative stress (OS) and ferroptosis. In this study, the Ca/Fe-based nanozymes are used as multi-enzyme simulants, which can effectively remove the reactive oxygen species and regulate ferroptosis to prevent and treat SAP. Notably, we make two trials for prevention and treatment of SAP. Under the condition of good biocompatibility, the Ca/Fe-based nanozymes effectively reduce the levels of serum pancreatitis-related biomarkers and inflammatory factors which involved in local and systemic inflammatory response. Moreover, the Ca/Fe nanozymes significantly increase the level of ferroptosis regulator of glutathione peroxidase 4 (GPx4) and ferritin heavy chain 1 (FTH1) in pancreas. These results demonstrate that the Ca/Fe-based nanozymes not only alleviate SAP but also mitigate subsequent multi-organ damage, thus providing an effective strategy of Ca/Fe nanozymes for treating SAP-related disorders in clinical research.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tong Zhang,Yuan Chen,Yurong Zhang,Bin Liu,Yuanyuan Liu,Jianwei Zhao
Cr(VI) and catechol are common pollutants in wastewaters of tannery industry. Cr(VI) reduction by catechol results in accumulation of Cr(V)-complex and toxic o -benzoquinone. Cr(VI) reduction can be enhanced by accelerating the electron transfer from catechol to Cr(VI) using Fe(III). This electron transfer allows the continuous production of reactive oxygen species (ROS) in advanced oxidation processes, which further degrades catechol. However, the effects of catechol on Fe(III)-based Cr(VI) reduction and ROS production are not clear. In this study, the electron transfer pathway between catechol, Fe(III) and Cr(VI) was investigated along with the catechol degradation by ROS. Results show that the process of Cr(VI) reduction follows well a pseudo-second-order kinetic model, and the activation energy decreases by 4189 J/mol after electrons are transferred by Fe(III). Aqueous chromium (50 mg/L) was completely precipitated as Cr(OH) 3 , Fe x Cr 1-x (OH) 3 or Fe(OH) 3 -Cr(OH) 3 at Fe(III) concentration of 10 mmol/L. Residual catechol and Fe(II) in wastewater activated percarbonate, thereby producing OH for over 480 min at pH 3.0 and generating OH and CO 3 − for over 5 min at pH 10.0. Catechol was degraded by these ROS to butenedioic, oxalic, and formic acids, which were then mineralized to H 2 O and CO 2 . Catechol (2 mmo/L) was fully removed from wastewater with TOC removal of 37%, and the degradation was not affected by SO 4 2− and Cl − . This study provides new insights into the removal of pollutants from wastewaters via electron transfer mediated by Fe(III), and may aid in controlling the toxic effects of Cr(VI) and catechol-like organics in natural and engineered aquatic systems.
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