Polymers
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2023
·Vol. 15
·期 19
·3879
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IF 5
Xiangyu Chen,Jiahua Ma,Xiaoshuai Sun,Chuanshan Zhao,Jiehua Li,Hui Li
This paper proposes a different strategy for deriving carbon materials from biomass, abandoning traditional strong corrosive activators and using a top−down approach with a mild green enzyme targeted to degrade the pectin matrix in the inner layer of pomelo peel cotton wool, inducing a large number of nanopores on its surface. Meanwhile, the additional hydrophilic groups produced via an enzymatic treatment can be used to effectively anchor the metallic iron atoms and prepare porous carbon with uniformly dispersed Fe−Nxstructures, in this case optimizing sample PPE−FeNPC−900’s specific surface area by up to 1435 m2g−1. PPE−FeNPC−900 is used as the electrode material in a 6 M KOH electrolyte; it manifests a decent specific capacitance of 400 F g−1. The assembled symmetrical supercapacitor exhibits a high energy density of 12.8 Wh kg−1at a 300 W kg−1power density and excellent cycle stability. As a catalyst, it also exhibits a half−wave potential of 0.850 V (vs. RHE) and a diffusion-limited current of 5.79 mA cm−2at 0.3 V (vs. RHE). It has a higher electron transfer number and a lower hydrogen peroxide yield compared to commercial Pt/C catalysts. The green, simple, and efficient strategy designed in this study converts abundant, low−cost waste biomass into high-value multifunctional carbon materials, which are critical for achieving multifunctional applications.Keywords:pomelo peel;enzymatic treatment;Fe−Nx;supercapacitors;ORR
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Chao Chen,Shilong Zhou,Jiawei Xia,Le Li,Xingyue Qian,Fengxiang Yin,Guangyu He,Haiqun Chen
Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N 4 sites anchored on N -doped hierarchically porous carbon (Fe-NC-C 3 N 4 ). The optimized Fe-NC-C 3 N 4 exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential ( E 1/2 ) of 0.90 V vs. RHE and a promising low overpotential of 0.305 V vs . RHE at 10 mA·cm −2 in alkaline electrolyte. These superior catalytic activities are attributed to the combined effect between the atomic active sites and the well-balanced micro-meso-macropore structures. The homemade liquid Zn-air battery (ZAB) assembled with Fe-NC-C 3 N 4 catalyst displays a power density of 133.59 mW·cm −2 and a significant energy density of 882.58 mAh·g −1 , exceeding those of the equipment with commercial Pt/C-RuO 2 (56.82 mW·cm −2 and 643.87 mAh·g −1 , respectively). Particularly, the corresponding flexible wearable ZAB manifests outstanding foldability and cyclical stability. This work opens a new perspective for the structural design of single-atom catalysts in the energy storage and conversion area.
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FUEL
·
2023
·
IF 7.4
Yuheng Qiao,Zhenzhen Guan,Mengyan Zhang,Gan Chen,Shifeng Zhou,Hailong Liu,Jiang Wu,Ruitang Guo,Weiguo Pan,Fangqin Li,Ping He
In this paper, a series of Fe-based catalysts with Zeolite Socony Mobil-5 (ZSM-5) as supports were synthesized using the sol–gel method to obtain the Fe/ZSM-5, Mn-Fe/ZSM-5, Cu-Fe/ZSM-5 and Cu-Mn-Fe/ZSM-5 catalysts. The synthesized catalysts were examined and characterized via catalytic activity testing, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N 2 adsorption/desorption, scanning electron microscope (SEM), temperature-programmed desorption of NH 3 (NH 3 -TPD), temperature-programmed reduction with H 2 (H 2 -TPR) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The results showed that the Cu-Mn-Fe/ZSM-5 catalyst had the best catalytic performance compared with the other catalysts. In addition, Fe/ZSM-5 and Cu-Mn-Fe/ZSM-5 all exhibited excellent stability as well as good tolerance to SO 2 & H 2 O under the experimental conditions. Further characterization results showed that with co-doping of Cu and Mn, the amount of Mn 4+ , Cu + , Fe 3+ and surface chemisorbed oxygen (O β ) on the surface of Fe/ZSM-5 increased, promoting the catalytic performance. The DRIFT studies revealed that the NH 3 -SCR reaction followed both the E-R and L-H mechanism on the surface of the Fe-based ZSM-5 catalyst. The Fe-based ZSM-5 catalyst is a good candidate for NH 3 -SCR both in high reactivity and outstanding stability.
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Nanomaterials
·
2023
·Vol. 13
·期 20
·2745
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IF 5.3
Jing Li,Mingjie Fan,Ziting Yuan,Fang Liu,Miao Li
Hexavalent chromium (Cr(VI)) is a typical heavy metal pollutant, making its removal from wastewater imperative. Although nanosized zero-valent iron (nZVI) and graphene-based materials are excellent remediation materials, they have drawbacks, such as agglomeration and being difficult to recycle. A facile synthesis method for decorating reduced graphene oxide (rGO) with ultrathin nZVI (within 10 nm) was explored in this study in order to develop an effective tool for Cr(VI) detoxication. Cu particles were doped in these composites for electron-transfer enhancement and were verified to improve the rate by 2.4~3.4 times. Batch experiments were conducted at different pHs, initial concentrations, ionic strengths, and humic acid (HA) concentrations. From these observations, it was found that the acid condition and appearance of Cu and rGO enhanced the treatment capacity. This procedure was fitted with a pseudo-second-order model, and the existence of NaCl and HA impeded it to some extent. Cr(VI) could be detoxified into Cr(III) and precipitated on the surface. Combining these analyses, a kinetics study, and the characterizations before and after the reaction, the removal mechanism of Cr(VI) was further discussed as a complex process involving adsorption, reduction, and precipitation. The maximum removal capacity of 156.25 mg g−1occurred in the acid condition, providing a potential Cr(VI) remediation method.Keywords:nano zero-valent iron (nZVI);reduced graphene oxide (rGO);Cu doping;hexavalent chromium (Cr(VI));removal
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Jimei Liu,Wenzhu Yu,Ziheng Zhao,Dong Liu,Shanshan Liu,Jie Wang,Mingliang Ma,Qinghua Yu,Naitao Yang
The unique layered structure and high conductivity of MXene materials make them highly promising for microwave absorption. However, the finite loss mechanism and severe agglomeration present challenging obstacles for ideal microwave absorbers, which could be effectively improved by constructing a three-dimensional (3D) porous structure. This study reports a 3D honeycomb MXene using a straightforward template method. The 3D MXene framework offers ample cavities to anchor the Prussian blue microcubes and their derivatives including Fe microboxes and Fe clusters by a simple annealing process. Based on the superiority of the 3D honeycomb architecture and magnetic–dielectric synergistic effects, the Fe/MXene absorbers demonstrate outstanding microwave absorption capabilities with the optimum reflection loss value of −40.3 dB at 2.00 mm in the low-frequency range from 4.2 to 5.6 GHz. The absorber also manifests superior radar wave attenuation by finite element analysis and exhibits great potential to be a flexible and thermal insulation material in a wide range of temperatures. This work proposes a useful reference for the design of 3D MXene-based porous architectures, and the synergistic magnetic–dielectric strategy further expands the potential of MXene-based absorbers, enabling them to be used as flexible and highly efficient microwave absorbers.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
YuXin Zhao,Jiaxian Liu,Tong Zhang,FangXun Liu,Man Zheng,Kun Shi,JinPeng Liu,Yufan Zhang,Huan Wang
The exploration of an inexpensive catalyst with effective oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) activities to replace precious metal electrocatalysts has been of great interest in recent years. In this paper, CNT@Co-Fe/FePc composites were synthesized with high efficiency using a self-assembly strategy. In the synthesis process, carbon nanotubes (CNTs) were synthesized as the base material using crab shells as templates and honey as the carbon and nitrogen source. CoFe alloy nanoparticles derived from CoFe-based prussian blue analogs were self-assembled and anchored on CNTs, and then iron phthalocyanine with Fe-N 4 portion was coupled with CNTs by π-π stacking. Finally formed a homogeneous and stable composite material. The self-assembly method is simple and efficient to achieve good metal loading. The prepared CNT@Co 2 -Fe 1 /FePc exhibits excellent catalytic performance and stability for OER and ORR in alkaline electrolyte . The overpotential at 10 mA cm −2 of CNT@Co 2 -Fe 1 /FePc for OER is 343 mV with a very small Tafel slope of 43.59 mV dec −1 . CNT@Co 2 -Fe 1 /FePc has high methanol tolerance and persistence for ORR. This work provides a strategy for the construction of transition metal-carbon composite electrocatalytic materials with excellent catalytic performance and stability for OER and ORR reactions.
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TALANTA
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2018
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IF 4.244
Qiumeng Chen,Chunhong Liang,Xiaodan Zhang,Yuming Huang
The N-doped porous carbon (NC) has been regarded as one of the promising support materials for nanoparticles (NPs) catalyst due to its inherent virtues such as porosity, large surface areas, and heteroatom incorporation. In this work, Fe/NC-800 hybrid was facilely prepared by uniform dispersion of in situ formed FeNPs onto NC-800 from carbonization of ZIF-8 at 800 °C for the first time. The optimized Fe/NC-800 catalyst was characterized by TEM , XPS and XRD. Compared with sole FeNPs and NC-800, the Fe/NC-800 catalyst exhibited an enhanced oxidase-like activity that could oxidize the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to the heavy blue without extra oxidants such as H 2 O 2 . The possible reason for the enhanced oxidase-like activity of the Fe/NC-800 was discussed on the basis of the experiments of radical scavengers , indicating the importance of superoxide (O 2 •- ) and singlet ( 1 O 2 ) in colorimetric reaction between TMB and Fe/NC-800 hybrid. Furthermore, the oxidase-like activity of Fe/NC-800 was significantly inhibited by dopamine (DA), leading to blue color fading. On this basis, a sensitive and selective colorimetric sensor was fabricated for the quantitative analysis of DA with a linear range of 0.01–40 μM and a low detection limit of 10 nM. The proposed colorimetric method was successfully applied to determine DA in human serum and injection samples, suggesting a promising application in biological analysis.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Wangjun Lin,Linfeng Peng,Hui Li,Tangfu Xiao,Jianqiao Wang,Nana Wang,Xiangting Zhang,Hanmo Zhang
Fe(II)-induced phase transformations of secondary iron minerals have attracted considerable attention due to their influence on antimony (Sb) mobility. However, Fe(II)-induced natural multicomponent secondary iron mineral (nmSIM) transformations and the corresponding repartitioning of Sb on nmSIM under acidic conditions upon Fe(II) exposure have not been systematically examined. Herein, we investigated the effect of Fe(II) on nmSIM mineralogy and Sb mobility in Sb(V)-bearing nmSIM at pH 3.8 and 5.6 at various Fe(II) concentrations over 15 d. The Sb(V)-bearing nmSIM phase transformation occurred under both strongly and weakly acidic conditions without Fe(II) exposure, while the presence of Fe(II) significantly intensified the transformation, and substantial amounts of intermediary minerals, including jarosite , ferrihydrite , lepidocrocite and fougerite, formed during the initial reaction stage, especially at pH 5.6. X-ray diffraction (XRD) analyses confirmed that goethite and hematite were the primary final-stage transformation products of Sb(V)-bearing nmSIM, regardless of Fe(II) exposure. Throughout the Sb(V)-bearing nmSIM transformation at pH 3.8, Sb release was inversely related to the Fe(II) concentration in the initial stage, and after maximum release was achieved, Sb was gradually repartitioned onto the nmSIM. No Sb repartitioning occurred in the absence of Fe(II) at pH 5.6, but the introduction of Fe(II) suppressed Sb release and improved Sb repartitioning on nmSIM. This transformation was conducive to Sb reimmobilization on Sb(V)-bearing nmSIM due to the structural incorporation of Sb into the highly crystalline goethite and hematite generated by the Sb(V)-bearing nmSIM transformation, and no reduction of Sb(V) occurred. These results imply that Fe(II) can trigger mineralogical changes in Sb(V)-bearing nmSIM and have important impacts on Sb partitioning under acidic conditions. These new insights are essential for assessing the mobility and availability of Sb in acid mine drainage areas.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,Baolin Hou
Zero-valent copper (Cu(0))-triggered hydrogen peroxide (Cu(0)/H 2 O 2 ) process was used to eliminate and mineralize contamination, while its oxidation efficacy was limited by the reaction of Cu(I) with O 2 . In this study, ferric ion (Fe(III)) was spiked into the Cu(0)/H 2 O 2 (Fe(III)/Cu(0)/H 2 O 2 ) system, and the degradation rate of paracetamol decreased from 24.9% to 95.4%. In the Fe(III)/Cu(0)/H 2 O 2 system, the reaction of Cu(0) and Cu(I) with Fe(III) expedited the conversion from Fe(III) to Fe(II). The reaction of Cu(I) with O 2 was weakened by the competition reaction between Cu(I) and Fe(III), promoting the generation of reactive oxygen species and increasing the utilization of Cu(0). The main reactive oxygen species for pH 4.0 was •OH and Fe(IV) with the contribution rate of •OH and Fe(IV) being 92.3% and 7.7%, but the dominant reactive oxygen species at pH 3.0 was only •OH in the Fe(III)/Cu(0)/H 2 O 2 process. Especially, the contribution of Fe(IV) rose and the contribution of •OH decreased, when the concentrations of 20–80 μmol/L Fe(III), 0.05–0.3 g/L Cu(0) and 50–300 μmol/L H 2 O 2 incremented. In the Fe(III)/Cu(0)/H 2 O 2 process.After we increased the pH of end solution to 7.0/7.5/8.0 and leaching, the total copper in reaction solution was under 6.4/3.3/1.5 μmol/L. In addition, Ni(II) (57.7%), Fe(II) (100%) and Mn(II) (72.4%) obviously enhanced the degradation of paracetamol in the Cu(0)/H 2 O 2 process.
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Acta Biomaterialia
·
2023
·
IF 9.7
Jiawu Yu,Yuchen Zhang,Liqi Li,Yang Xiang,Xuemei Yao,Youbo Zhao,Kaiyong Cai,Menghuan Li,Zhongjun Li,Zhong Luo
Radiotherapy is a mainstream modality for breast cancer treatment that employs ionizing radiation (IR) to damage tumor cell DNA and elevate ROS stress, which demonstrates multiple clinically-favorable advantages including localized treatment and low invasiveness. However, breast cancer cells may activate the p53-mediated cell cycle regulation in response to radiotherapy to repair IR-induced cellular damage and facilitate post-treatment survival. F-Box and WD Repeat Domain Containing 7 (FBXW7) is a promoter of p53 degradation and critical nexus of cell proliferation and survival events. Herein, we engineered a cooperative radio-ferroptosis-stimulatory nanomedicine through coordination-driven self-assembly between ferroptosis-inducing Fe 2+ ions and FBXW7-inhibiting DNAzymes and further modification of tumor-targeting dopamine-modified hyaluronic acid (HA). The nanoassembly could be selectively internalized by breast cancer cells and disintegrated in lysosomes to release the therapeutic payload. DNAzyme readily abolishes FBXW7 expression and stabilizes phosphorylated p53 to cause irreversible G2 phase arrest for amplifying post-IR tumor cell apoptosis. Meanwhile, the p53 stabilization also inhibits the SLC7A11-cystine-GSH axis, which combines with the IR-upregulated ROS levels to amplify Fe 2+ -mediated ferroptotic damage. The DNAzyme-Fe-HA nanoassembly could thus systematically boost the tumor cell damaging effects of IR, presenting a simple and effective approach to augment the response of breast cancer to radiotherapy. Statement of Significance To overcome the intrinsic radioresistance in breast cancer, we prepared co-assembly of Fe 2+ and FBXW7-targeted DNAzymes and modified surface with dopamine conjugated hyaluronic acid (HA), which enabled tumor-specific FBXW7-targeted gene therapy and ferroptosis therapy in IR-treated breast cancers. The nanoassembly could be activated in acidic condition to release the therapeutic contents. Specifically, the DNAzymes could selectively degrade FBXW7 mRNA in breast cancer cells to simultaneously induce accumulation of p53 and retardation of NHEJ repair , eventually inducing irreversible cell cycle arrest to promote apoptosis. The p53 stabilization would also inhibit the SLC7A11/GSH/GPX4 axis to enhance Fe 2+ mediated ferroptosis. These merits could act in a cooperative manner to induce pronounced tumor inhibitory effect, offering new approaches for tumor radiosensitization in the clinics.
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ACS Applied Nano Materials
·
2023
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IF 5.9
Yao Shen,Siqi He,Yongyue Zhuang,Shuchen Huang,Chunfeng Meng,Aihua Yuan,Wenhua Miao,Hu Zhou
One-dimensional metal/N-doped carbons have exhibited promise for use as efficient catalysts of the oxygen reduction reaction (ORR). In this work, Fe,N-doped carbon nanotubes (Fe-NC@NCNT) are developed by pyrolyzing the precursor/template of a polypyrrole (PPy) nanotube-anchored Fe/Zn-based zeolite imidazole framework. Thanks to the hierarchical tubular nanostructure, high electronic conductivity, and abundant Fe-based species (Fe-Nx sites and Fe/Fe3C nanoparticles), the designed electrocatalyst exhibits a catalytic property comparable to that of commercial Pt/C. Specifically, the Fe-NC@NCNT catalyst undergoes a four-electron ORR pathway with an onset potential of 0.96 V and a half-wave potential of 0.88 V versus reversible hydrogen electrode, a small Tafel slope of 60.0 mV dec–1, remarkable long-term cycle durability, as well as strong alcohol tolerance in an alkaline electrolyte. When applied to the air-electrode catalyst of rechargeable zinc–air batteries, the Fe-NC@NCNT-catalyzed liquid-state battery delivers an open-circuit voltage of 1.44 V and a maximum power density of 115 mW cm–2 with a specific capacity of 814 mAh g–1, outperforming those of the battery assembled with commercial Pt/C + RuO2. In addition, the as-assembled solid-state battery displays a desirable rechargeability and electrochemical flexibility. The present study establishes a facile dual-template approach to fabricate highly efficient and inexpensive ORR electrocatalysts toward the application of metal–air batteries.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Lingxiang Huang,Yue Ma,Mufan Niu,Shenyong Ren,Qiaoxia Guo,Chunming Xu,Baojian Shen
Dry reforming reaction of greenhouse gas CH 4 and CO 2 was studied over Ni-Fe bimetallic catalyst, in which the composite support of C12A7-O 2- in MCM-41 was used. The isotope 13 CH 4 /D 2 O tracing experiment showed CO mainly comes from 13 CHx oxidation reaction and DH comes from CHx and D 2 O reaction, exhibiting lattice oxygen promotes CH X oxidation and water accelerate methane conversion. XPS and TPSR-MS studies exhibited the existence of lattice oxygen in catalysts produces a little H 2 O to facilitate a lower starting point at the reaction temperature. On-line MS investigation found that the trace water addition in the system accelerated the adsorption of CO 2 on support and promoted methane dissociation, the H 2 signal appears later than CO, indicating the oxidation reaction of CHx occurs after the dissociation of CO 2 . Besides, TG analysis tells us the H 2 O may consume Cα on the catalyst in time during the reaction process to remove carbon deposition.
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