ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lei Jia,Linwen Jiang,Jiawen Hu,Jiawei Jin,Siqin Yan,Anhua Wu,Xiaofeng Zhang
Optimizing the impedance matching via electromagnetic adjustment is considered an effective strategy to accomplish exceptional electromagnetic wave absorption (EMA) performance. Here, we report an efficient and green process to obtain the carbonitriding FeCoNiCr high-entropy alloys (HEAs) with flake-shaped morphology by using organic cyanide (Dicyandiamide, C2H4N4) as nitrogen and carbon sources. The carbonitriding effects on the phase structure, magnetic properties, mechanical hardness, corrosion resistance, high-temperature oxidation resistance, and EMA performances were investigated systematically. The carbonitriding process optimized the impedance match by decreasing the dielectric constant via introducing the nonmetallic C and N. The #CN10 sample exhibited outstanding EMA performances with a minimum reflection loss of −32.3 dB at 7.89 GHz and a broad effective bandwidth of 4.46 GHz, which covered the majority of X-band. In addition, the carbonitriding FeCoNiCr HEAs had great mechanical properties, excellent corrosion resistance, and high-temperature oxidation resistance, indicating excellent adaptability to harsh environments as well as good EMA performances. This work provides a new idea for the preparation and design of carbonitriding EMA materials.
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Nano Research
·
2023
·
IF 9.9
Dong Zhicheng,Xu Yunyun,Wu Can,Chao Jin,Tian Chen,Lin Zhang
Organo-chromium(III) complex is one of the chromium contaminant species, which would transform to high-toxic Cr(VI) during migrating in the environment. Such natural organo-chromium(III) (NOCr) is difficult to remove by traditional degradation or precipitation methods, due to its high stability and solubility. Herein, we demonstrated a novel NOCr removing method by transforming it to certain structures similar to Cr-Fe minerals in nature, through a self-circulating decomplex and immobilization mechanism with nano zero-valent iron (nZVI). Taking chromium glycinate (Cr-Gly) as a probe, nZVI showed a high Cr removal efficiency of 99.4% under ambient conditions. The removal process included three stages of adsorption, decomplexation, and re-immobilization. Cr-Gly was first adsorbed on the surface of nZVI by chemisorption of the oxide shell. Then, the adsorbed Cr-Gly was decomplexed and oxidized to Cr(VI) by ·OH and 1 O 2 , which were generated from molecular oxygen activated by nZVI. Meanwhile, the released Cr(VI) could be in-situ adsorbed and re-reduced to Cr(III), which was further immobilized in form of Cr-O-Fe complex. As the Cr-O-Fe complexing structure was similar to that of Cr-Fe minerals (such as chromohercynite) in nature, this work explored a novel and efficient NOCr removing method that was potential to weaken chromium pollution in the environment.
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ENERGY & FUELS
·
2023
·
IF 5.3
Xianhang Jin,Enze Ren,Min Zheng,Xiurong He,Yun Yang
A CO2 phase change absorbent (CPCA) is of interest because it has the potential to reduce energy consumption for CO2 capture. Controllable phase separation behavior was expected in the development and application of a CPCA. In this study, the effects of CO2 loading under different activators and physical solvents on the phase separation behavior of an activated methyldiethanolamine (MDEA)-based CPCA were investigated. By adjustment of the CO2 loading, controllable phase separation behavior was achieved and the absorbent comprising an activator with more −NH– groups and a physical solvent with low ET(30) was favored to exhibit phase separation. Of special interest was that, with the increasing of CO2 loading, phase behaviors, from the liquid phase to solid–liquid phase and then to the liquid phase, were observed for CPCA comprising MDEA/piperazine (PZ)/N-methyl-2-pyrrolidone (NMP), which was different from all of the other known CPCAs. The solid compound was identified as PZ carbamate by X-ray diffraction (XRD), Fourier transform infrared (FTIR), and elemental analysis, and the liquid-phase samples were detected by 13C nuclear magnetic resonance (NMR). The phase change mechanism of this special phenomenon was proposed.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Ludi Song,Lvren Lin,Wenjia Wei,Shengkun Zhang,Lei Wan,Zimo Lou,Jianming Yu,Xinhua Xu
Mechanochemical (MC) remediation with zero-valent iron (ZVI) as co-milling agent enables the non-combustion and solvent-free disposal of solid halogenated organic pollutants (HOPs) via solid-phase reaction, but suffers from incomplete dechlorination (especially for less chlorinated chemicals). Herein, a reduction-oxidation coupling strategy using ZVI and peroxydisulfate as synergistic (ZVI-PDS) co-milling agents was investigated, with 2,4-dichlorophenol (2,4-DCP) as probe contaminant. By revisiting the MC destruction process of 2,4-DCP by ZVI, the contribution of both reductive and oxidative routes is confirmed, and the inefficient •OH generation is addressed. With ball-to-material and reagent-to-pollutant mass ratios of 30:1 and 13:1, respectively, ZVI-PDS achieves higher dechlorination ratio (86.8%) for 2,4-DCP within 5 h, outcompeting sole ZVI (40.3%) or PDS (33.9%), due to the accumulation of numerous SO 4 •− . As suggested by a two-compartment kinetic model , the optimal ZVI/PDS molar ratio of 4:1 is determined, which balances the relative contribution of reductive/oxidative routes and leads to a maximum mineralization efficiency of 77.4%. The analysis on product distribution verifies the generation of dechlorinated, ring-opening and minor coupling products (with low acute toxicity). This work validates the necessity to couple reduction with oxidation in MC destruction for solid HOPs, and may provide information on reagent formulation.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Chengjie Xue,Yunqiang Yi,Long Zhou,Zhanqiang Fang
The problem of co-contaminated soil at e-waste dismantling sites is serious and constitutes a critical threat to human health and the ecological environment. Zero-valent iron (ZVI) has been proven to be effective in the stabilization of heavy metals and the removal of halogenated organic compounds (HOCs) from soils. However, for the remediation of co-contamination of heavy metals with HOCs, ZVI has disadvantages such as high remediation cost and inability to take into account both pollutants, which limits its large-scale application. In this paper, boric acid and commercial zero-valent iron (cZVI) were used as raw materials to prepare boric acid-modified zero-valent iron (B-ZVI bm ) through a high-energy ball milling strategy. B-ZVI bm coupled with persulfate (PS) to achieve simultaneous remediation of co-contaminated soil. The synergistic treatment of PS and B-ZVI bm resulted in the removal efficiency of 81.3% for decabromodiphenyl ether (BDE209) and the stabilization efficiencies of 96.5%, 99.8%, and 28.8% for Cu, Pb, and Cd respectively in the co-contaminated soil. A series of physical and chemical characterization methods showed that the oxide coat on the surface of B-ZVI bm could be replaced by borides during ball milling. The boride coat facilitated the exposure of the Fe 0 core, promoted the corrosion of ZVI and the orderly release of Fe 2+ . The analysis of the morphological transformation of heavy metals in soils revealed that most of the heavy metals in the exchangeable, carbonate-bound state were transformed into the residue state, which was the key mechanism for the remediation of heavy metal-contaminated soils with B-ZVI bm . The analysis of BDE209 degradation products showed that BDE209 was degraded to lower brominated products and further mineralized by ZVI reduction and free radical oxidation . In general, B-ZVI bm coupled with PS is a good recipe for synergistic remediation of co-contaminated soils with heavy metals and HOCs.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 43
·2303832
·
IF 19
Shuo Chen,Yongkang Lyu,Yang Sun,Qin Wei,Chuansong Chen,Lei Chen,Xinhao Zhang,Heqi Ma,Tianyu Sun,Wen Gao,Yazhe Xu,Baoyuan Man,Qingtian Meng,Cheng Yang
Graphene field-effect transistors (G-FETs) have attracted widespread attention in disease diagnosis, benefiting from these advantages of high sensitivity, label-free, easy integration, and direct detection of nucleic acids (NAs) in liquid environments. However, the problem of nonspecific signals in G-FETs is not fundamentally solved due to a lack of systematic theoretical research to support the development of effective solutions. Thus, researchers have to rely on speculative mechanisms to minimize nonspecific signals in experiments as much as possible. Herein, the nonspecific signal mechanism caused by eight types of π – π interaction paths mediated by aromatic rings is theoretically determined. Based on theoretical simulation results, the feasibility of blocking nonspecific signal paths through Nafion functionalization methods is experimentally verified. Experiments confirm that Nafion-modified G-FETs (NMG-FETs) have excellent performance in avoiding nonspecific signals compared to traditional G-FETs. Furthermore, the NMG-FET achieves ultra-sensitive detection of Down syndrome–related DNA down to 1 aM and severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA down to 5 aM, and shows good specificity in base recognition. This study is expected to promote the theoretical advancement of the nonspecific signal mechanism in G-FET NA detection and offer a practical strategy for improving signal purity and accuracy.
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POLYMERS FOR ADVANCED TECHNOLOGIES
·
2023
·Vol. 34
·期 10
·3125-3136
·
IF 3.4
Longwei Shi,Zheng Zhao,Lishuai Zong,Jinyan Wang,Xigao Jian
Limiting molecules' polarized motion effectively reduces the dielectric loss of materials. This article synthesized side chains with different lengths using p-ethoxyphenol, p-hydroxybenzoic acid, and long-chain halohydrins through a two-step process. These chains' movement was almost unaffected by the main chain of polymers, so they can fill up the free volume of polymers under certain conditions. 1,2-dihydro-4-(4-hydroxyphenyl)phthalazine-1-(2H)-one(DHPZ), 4,4'-Difluorophenyl sulfone(DFS), and 4,4-Bis(4-hydroxyphenyl) valeric acid(HPV) obtained three polymers with different carboxyl groups (10%, 30%, and 50%) through nucleophilic substitution. They were then grafted and treated with hot-pressing. The introduction of side chains could reduce the free volume of polymers under hot-pressing conditions, so further reducing the dielectric loss of materials. Polymer with the shortest and least (10%) side chains showed the most obvious dielectric loss tangent, the reduction rate of the film's dielectric loss tangent was 13.11% (at T g + 15°C, while the non-grafted one was only 3.69%) and 20.70% (at T g + 80°C, while the non-grafted one was only 8.35%), respectively. In addition, WXRD and DMA tests showed that films' intermolecular chain spacing (“ d ”) and T g changed after the hot-pressing process, respectively. The change law of both was consistent with that of dielectric loss tangent. Confirm that grafting high-motility side chains can significantly reduce polymer's dielectric loss by enhancing the free volume reduction effect after hot-pressing.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shiyang Li,Longdou Tu,Yeqiang Lu,Mingjie Lin,Junmei Ma,Chaojie Bai,Congjie Gao,Lixin Xue
A novel strategy was developed to build high-performance thin film composite (TFC) total heat exchange membranes (THEMs) by in situ growing ZIF-8 crystalline micro-leaves (ZIF-L) from Polyethyleneimine (PEI) coated on polysulfone (PSF) ultra-filtration substrates. It was found that flexible PEI polymeric chains could tightly cross-link and seal large masses of ZIF-L micro-leaves (ZIF/PEI wt. ratio up to 18.5) to thwart CO 2 permeation, on top of PSF substrate. Such PEI cross-linking could also effectively open up the internal channels of ZIF-L micro-leaves to enhance moisture permeance and latent heat recovery without trading off CO 2 gas barring property. ZIF-L in varied shapes protruded into the air stream could provide ultra-rough surfaces with increased surface area for improved total energy recovery efficiency. Optimized PEI/ZIF-L TFC THEMs showed ultra-low CO 2 permeance of 0.5–8 GPU and ultra-high total heat recovery rates of 68–74%.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jianxiong Gao,Longbin Zhang,Zhiqiang Xu,Xianxian Sheng,Dexiao Li,Yuantian Chen,Mudassir Habib,Shuguang Lyu
In this research, zero-valent iron (ZVI) was chosen as a reductant in the classic Fenton system to accelerate the generation of Fe(II). The removal of 1,2,3-trichloropropane (TCP) was only 65.3% in classic Fenton system, while with the addition of ZVI its removal could be enhanced to 95.4% in 120 min. Hydroxyl radicals (HO•) was confirmed to be the major radical during TCP degradation by electron paramagnetic resonance (EPR) detection and radical quenching tests. Moreover, the mechanism of TCP degradation in H 2 O 2 /Fe(II)/ZVI system was proposed. In the presence of ZVI, Fe(III) was reduced to Fe(II), further reacted with H 2 O 2 and produced more HO• for TCP removal. 2,3-Dichloro-1-propene and 2-chloro-2-propen-1-ol were the main intermediates in TCP degradation and two possible pathways were proposed. Finally, TCP removal in different solution matrixes and for other chlorinated contaminants removal were tested, revealing the broad-spectrum reactivity and excellent performance of ZVI-enhanced Fenton system in the remediation of chlorinated organic compounds.
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npj Materials Degradation
·
2023
·Vol. 7
·期 1
·1-10
·
IF 5.1
Yang Jingzhi,Ran Yami,Huang Luyao,Ren Chenhao,Hao Xiangping,Ma Lingwei,Zhang Dawei
2-hydroxyethyl methacrylate (HEMA), poly(ethylene glycol) (PEG), and zwitterionic polymers are currently considered the most extensively studied antifouling hydrogel coatings. However, systematic identification of these coatings to unleash their potential properties is tremendously under-represented. Here, we report a high-throughput optimizing strategy that combines highly miniaturized hydrogel synthesis and screening to fine design zwitterion-based hydrogel coatings. Compared with the traditional one-by-one synthesis and characterization methods, the proposed high-throughput strategy accelerated the discovery of candidate materials with a high-efficiency and cost-effective approach. To tailor multiple parameters of coatings, 1575 unique coating combinations with continuous gradients were prepared only required 600 μL reactant. The mechanical stability and drug-loading capacity of the coating spots were sequentially evaluated via immersion swelling, flow, tape-peeling, and dye-retaining tests. This strategy could efficiently reveal the composition/structure-function relationships of the hydrogel coatings and also other materials, which is promising for the rapid screening and design of desired implantable device surfaces.
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LANGMUIR
·
2023
·
IF 3.9
Qing Qing,Xian-ying Shi,Shao-zhong Hu,Liang Li,Ting Huang,Nan Zhang,Yong Wang
Increasing environmental problems intensify the demand for high-performance environmental purification materials. MXene is a typical transition-metal carbide/nitride material with a two-dimensional geometric feature and a good deal of functional groups, and it is considered as an efficient adsorbent for removing pollutants from wastewater. However, the easy oxidation and relatively low adsorption capacity greatly restrict its application. In this study, the MXene/polydopamine (PDA) composite particles were fabricated through the biomimetic modification method of inducing the self-polymerization of dopamine in an MXene aqueous solution. Microstructure characterizations demonstrate that PDA facilitates the exfoliation of MXene. Adsorption measurements show that MXene and PDA exhibit an apparent synergistic effect in removing chromium hexavalent Cr(VI) from aqueous solution, and more PDA content leads to a larger synergistic effect. Consequently, the composite particles exhibit an ultrahigh adsorption capacity (862.3 mg/g). Specifically, even if the composite particles were stored in aqueous solution for 2 months, they still exhibit high adsorption ability with only a 3.3% loss in adsorption capacity, indirectly confirming the enhanced stability of MXene induced by PDA. Furthermore, the composite particles also show reduction ability to Cr(VI) and about 54.3% Cr(VI) can be reduced to harmless chromium trivalent Cr(III). This study provides a new method for the preparation of MXene-based adsorbents with excellent adsorption capacity and high stability, which has broad application prospects in the field of wastewater treatment.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ying Chu,Peng Wang,Yihong Ding,Jie Lin,Xinxin Zhu,Shiqiang Zhao,Huile Jin,Tianbiao Zeng
Antimony (Sb) has been considered a promising anode for sodium-ion batteries (SIBs) owing to its high theoretical capacity (660 mA h g–1) and low redox voltage (0.2–0.9 V vs Na+/Na). However, the capacity degradation caused by the volumetric variation during battery discharge/charge hinders the practical application. Herein, guided by the DFT calculation, Sb/Fe2S3 was fabricated by annealing Fe and Sb2S3 mixed powder. Next, Sb/Fe2S3 was blended with 15 wt % graphite by ball milling, yielding nano-Sb/Fe2S3 anchored on an exfoliated graphite composite (denoted as Sb/Fe2S3-15%). When applied as an anode of SIBs, Sb/Fe2S3-15% delivered reversible capacities of 565, 542, 467, 366, 285, and 236 mA h g–1 at current rates of 1, 2, 4, 6, 8, and 10 A g–1, respectively, surpassing most of the Sb-based anodes. The co-existence of highly conductive Fe2S3 and Sb minimizes the polarization of the anode. Our experiments proved that the Sb and Fe2S3 phases were reversible during discharge/charge cycling, and the exfoliated graphite can accelerate the Na+ diffusion and e– conduction. The proposed synthesis method of this work can also be applicable to synthesize various antimony/transition metal sulfide heterostructures (Sb/M1–xS), which may be applied in a series of fields.
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