Materials Today Communications
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2023
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IF 3.8
Jianye Shi,Jin Chen,Xinle Wang,Zhikang Liu,Yuzhao Ma,Xiaofeng Yang,Meidan Que,Yanjun Li
Developing a lightweight microwave absorbing materials with high absorption capacity and wide absorption bandwidth at low thickness is a perennial challenge in practical applications in the microwave absorption (MA) field. Herein, sandwich-like heterogeneous Ti 3 C 2 T x /TiO 2 /Fe 3 O 4 /Fe are designed by synergistically incorporating dielectric-magnetic components with a simple solvothermal method and post-annealing. The sandwich-like heterogeneous interface produces sufficient conduction loss for Ti 3 C 2 T x /TiO 2 /Fe 3 O 4 /Fe, with TiO 2 crystals and amorphous carbon anchored on its surface to enhance interface polarization and Debye relaxation. Additionally, the presence of Fe nanoparticles induces magnetic loss, including natural resonance and eddy current loss. By bidirectionally regulating the ratio of Ti 3 C 2 T x and Fe 3 O 4 , the minimum reflection loss (RL min ) value reaches − 64.6 dB at 17.49 GHz with a 1.48 mm thickness, and the corresponding effective absorption bandwidth (EAB, RL < −10 dB) is 4.59 GHz (13.41–18 GHz). The results suggest that the exceptional EMW absorption performance of composites can be attributed to the dielectric-magnetic synergistic effect and sandwich-like heterostructures . This study offers a rational approach for synthesizing ultrathin and lightweight Ti 3 C 2 T x -based absorbers.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
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IF 4.3
Chu Shushu,Xia Mingyuan,Xu Peng,Lin Dalei,Jiang Yuanyuan,Lu Yizhong
Although traditional Fe-based nanozymes have shown great potential, generally only a small proportion of the Fe atoms on the catalyst’s surface are used. Herein, we synthesized single-atom Fe on N-doped graphene nanosheets (Fe-CNG) with high atom utilization efficiency and a unique coordination structure. Active oxygen species including superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ) were efficiently generated from the interaction of the Fe-CNG with dissolved oxygen in acidic conditions. The Fe-CNG nanozymes were found to display enhanced oxidase-like and laccase-like activity, with V max of 2.07 × 10 −7 M∙S −1 and 4.54 × 10 −8 M∙S −1 and K m of 0.324 mM and 0.082 mM, respectively, which is mainly due to Fe active centers coordinating with O and N atoms simultaneously. The oxidase-like performance of the Fe-CNG can be effectively inhibited by ascorbic acid (AA) or hydroquinone (HQ), which can directly obstruct the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB). Therefore, a direct and sensitive colorimetric method for the detection of AA and HQ activity was established, which exhibited good linear detection and limit of detection (LOD) of 0.048 μM and 0.025 μM, respectively. Moreover, a colorimetric method based on the Fe-CNG catalyst was fabricated for detecting the concentration of AA in vitamin C. Therefore, this work offers a new method for preparing a single-atom catalyst (SAC) nanozyme and a promising strategy for detecting AA and HQ.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Desen Zhou,Xuan Zhang,Zheng Li,Jun Zhang,Tielin Wang,Shaowen Cao
Photocatalytic conversion of CO 2 to usable fuels provides a new strategy for solving energy problems and the greenhouse effect. Porphyrin-based metal-organic frameworks (MOFs) are promising in photocatalysis due to their remarkable light harvesting ability, and the metal active site and its coordination environment can be further adjusted to achieve the high activity. In this work, g-C 3 N 4 /PCN-222 composites with different porphyrin metal centers were fabricated and the g-C 3 N 4 /PCN-222(Fe III ) catalyst showed the highest photocatalytic CO 2 reduction performance than that of g-C 3 N 4 /PCN-222(Fe II ) and other g-C 3 N 4 /PCN-222( M , M = Co, Ni, Cu, Zn) composites. Experimental studies and theoretical calculations showed that the axial coordination in g-C 3 N 4 /PCN-222(Fe III ) distorts the square planar field (Fe-N4) to quasi-octahedral coordination, which led to the moderate adsorption ability of CO 2 reduction intermediate (*CO), resulting in the high photocatalytic activity.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Katam Srinivas,Zhuo Chen,Anran Chen,Fei Ma,Ming-qiang Zhu,Yuanfu Chen
The development of efficient single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) remains a formidable challenge, primarily due to the symmetric charge distribution of metal single-atom sites (M-N 4 ). To address such issue, herein, Fe-N x sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution, thus enhancing the intrinsic catalytic activity. Precisely, atomically dispersed Fe-N x sites supported on N/S-doped mesoporous carbon (NSC) coupled with FeS@C core-shell nanoparticles (FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis. Due to the presence of an in situ-grown conductive graphitic layer (shell), the FeS nanoparticles (core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions. Consequently, FAS-NSC@950 displays a more positive half-wave potential ( E 1/2 ) of 0.871 V with a significantly boosted ORR kinetics (Tafel slope = 52.2 mV dec −1 ), outpacing the commercial Pt/C ( E 1/2 = 0.84 V and Tafel slope = 54.6 mV dec −1 ). As a bifunctional electrocatalyst, it displays a smaller bifunctional activity parameter (Δ E ) of 0.673 V, surpassing the Pt/C-RuO 2 combination (Δ E = 0.724 V). Besides, the FAS-NSC@950-based zinc-air battery (ZAB) displays superior power density, specific capacity, and long-term cycling performance to the Pt/C-Ir/C-based ZAB. This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR, with potential implications for energy conversion and storage technologies.
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INORGANIC CHEMISTRY
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2023
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IF 4.6
Yulu Wu,Yanning Qu,Chenyang Su,Xiufang Yang,Yuhao Yang,Yanan Zhang,Wenhuan Huang
Single-atom metal-anchored porphyrin-based metal–organic frameworks (MOFs) have shown excellent light absorption, catalytic sites, and high stability during photocatalytic reactions, while there are still challenges for facile assembly with quantum dots to enhance catalytic dynamics. Herein, a kind of Fe single atom-doped MOF material (Fe-MOF-525) was ball milled with CdS in a proper ratio through Fe–N4 and Fe–N–C bonding, which showed the enhanced photoinduced carrier separation ability. As a result, extended light absorption ranges of CdS/Fe-MOF-5252.3 induced the promotion of the photocatalytic hydrogen (H2) value (3638.6 μmol g–1 h–1), which was 7.2 and 2.3 times higher than those of Fe-MOF-525 and CdS. In this work, the facile synthetic technique, specific active sites, and enhanced catalytic dynamics in the composite highlight the future research on MOF-based heterojunctions and their potential photocatalysis applications..
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MOLECULES
·
2023
·Vol. 28
·期 22
·7591
·
IF 4.6
Jian Huang,Yu Zhu,Huiyang Bian,Liang Song,Yifan Liu,Yuancai Lv,Xiaoxia Ye,Chunxiang Lin,Xiaojuan Li
A boron and iron co-doped biochar (B-Fe/biochar) from Masson pine bark was fabricated and used to activate peroxydisulfate (PDS) for the degradation of guaiacol (GL). The roles of the dopants and the contribution of the radical and non-radical oxidations were investigated. The results showed that the doping of boron and iron significantly improved the catalytic activity of the biochar catalyst with a GL removal efficiency of 98.30% within 30 min. The degradation of the GL mainly occurred through the generation of hydroxyl radicals (·OHs) and electron transfer on the biochar surface, and a non-radical degradation pathway dominated by direct electron transfer was proposed. Recycling the B-Fe/biochar showed low metal leaching from the catalyst and satisfactory long-term stability and reusability, providing potential insights into the use of metal and non-metal co-doped biochar catalysts for PDS activation.Keywords:Masson pine bark;biochar;peroxydisulfate activation;B/Fe co-doping
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WATER RESEARCH
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2023
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IF 12.8
Yu Wang,Yanchun Deng,Lu Yao,Xin Yang
The omnipresence of natural organic matter (NOM) in water bodies traditionally hinders the degradation of trace organic contaminants (TrOCs) in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). This study elucidates the positive role of NOM in enhancing the degradation of TrOCs through the Fe(III)/PMS process. During this process, NOM reduces Fe(III), yielding semiquinone-like radical (NOM • ) and concurrently forming NOM-Fe(III) colloids. In addition to the Fe(II)-mediated activation pathway, Fe(III) sites on NOM-Fe(III) colloids effectively transfer electrons from NOM • or some redox-active moieties to PMS, resulting in the generation of long-lived colloid-bound SO 4 •− , which can readily undergo hydrolysis to produce HO • . The stabilization of SO 4 •− and HO • by NOM-Fe(III) colloids, combined with their moderate adsorption of TrOCs, results in surface-confined reactions that significantly enhance TrOC removal, despite the presence of concurrent quenching reactions between radicals and NOM. Further, the significant positive correlation between the phenolic contents of eight NOM types and TrOC degradation kinetics suggests phenolic moieties as the primary electron source for PMS activation. By in-situ utilizing NOM in raw water, a PMS-amended iron coagulation process with 0.2 mM Fe(III) and PMS effectively removes 90–100 % of six coexisting TrOCs. This study unveils the previously unrecognized role of colloid-bound radicals in decontamination processes, offering valuable insights into harnessing NOM's influence in advanced oxidation water treatment processes.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Xuefeng Wu,Jinyuan Zhu,Waseem Hayat,Yongqing Zhang,Shaobin Huang,Ran Jiang
An iron (Fe)-modified carbon dots (CDs) doped ZIF-8 zeolite imidazole metal-organic frame pyrolyzed composite (5Fe@NC) was prepared and then evaluated as a peroxydisulfate (PDS) activator for the oxidative removal of organic pollutants . The 5Fe@NC/PDS system not only has a good recovery performance, wide pH adaptability, and low activation energy, but also is resistant to environmental interference. The quenching experiments, electron paramagnetic resonance (EPR) detection, and electrochemical analysis all revealed that unlike the widely reported singlet oxygen ( 1 O 2 ) dominated nonradical mechanism, an electron transfer process (ETP) involving a surface bound PDS complex played the main role in pollutants’ degradation by 5Fe@NC/PDS system. The FeN x , defect, graphitic N and hydroxyl group (-OH) acting as active sites, prompted the 5Fe@NC-PDS complex to capture electrons (e − ) from acetaminophen (ACT). This study provides a new approach for xFe@NCs rational design, and deepen the understanding of FeN x activation mechanism of PDS in carbon nanomaterials .
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
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IF 16.6
Wei Shengjie,Sun Yibing,Qiu Yun-Ze,Li Ang,Chiang Ching-Yu,Xiao Hai,Qian Jieshu,Li Yadong
Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N 4 sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N 4 sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N 4 sites.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jing Wei,Zhigang Zheng,Lin Zhao,Zhaoguo Qiu,Dechang Zeng
A method involving the application of an elevated proton conductive shell onto Fe-base amorphous alloys (Fe am ) through the mechanical ball-milling process with oxalic acid dihydrate (OA-BFe am ) is presented. The investigation highlights that the resulting Fe 2 C 2 O 4 ·shell remarkably enhances the removal rate of acid orange II (AO II) by Fe am , exhibiting an approximately 2.17-fold increase. This enhancement is attributed to the superior proton conductivity of the Fe 2 C 2 O 4 shell in comparison to the iron oxide shell. Consequently, protons can effectively traverse the Fe 2 C 2 O 4 shell and permeate into the iron core, where they serve as reducing agents to generate H. Simultaneously, the formation of surface-adsorbed Fe 2+ occurs rapidly, contributing to a highly efficient AO II removal process across a broad pH range. Additionally, it is noteworthy that OA-BFe am exhibits equivalent efficacy in the removal of both direct and reactive dyes. Overall, this work introduces an environmentally benign surface modification technique for Fe am and underscores the influence of proton conductivity on the dye wastewater removal capability of Fe am .
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Small
·
2023
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IF 13.3
Qiusheng Zhou,Min Min,Minmin Song,Shiqiang Cui,Nan Ding,Mingyuan Wang,Shuangying Lei,Chuanyin Xiong,Xinwen Peng
The rational design of bifunctional oxygen electrocatalysts with unique morphology and luxuriant porous structure is significant but challenging for accelerating the reaction kinetics of rechargeable Zn–air batteries (ZABs). Herein, zinc-mediated Fe, N-codoped carbon nanocages (Zn-FeNCNs) are synthesized by pyrolyzing the polymerized iron-doped polydopamine on the surface of the ZIF-8 crystal polyhedron. The formation of the chelate between polydopamine and Fe serves as the covering layer to prevent the porous carbon nanocages from collapsing and boosts enough exposure and utilization of metal-based active species during carbonization. Furthermore, both the theoretical calculation and experimental results show that the strong interaction between polyhedron and polydopamine facilitates the evolution of high-activity zinc-modulated FeNx sites and electron transportation and then stimulates the excellent bifunctional catalytic activity for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). As expected, the Zn–air battery with Zn-FeNCNs as an air cathode displays a superior power density (256 mW cm −2 ) and a high specific capacity (813.3 mA h gZn −1 ), as well as long-term stability over 1000 h. Besides, when this catalyst is applied to the solid-state battery, the device exhibited outstanding mechanical stability and a high round-trip efficiency under different bending angles.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Xiaowei Liu,Peng Chen,Xiangdong Li,Jiaen Zhong,Kexin Li,Miaomiao Ye,Lili Wang
The widespread implementation of ultrafiltration (UF) technology, which has gained popularity for drinking water treatment, has been impeded by rising operational costs and shortened membrane lifespans resulting from membrane fouling. Here, an integrated pretreatment technique combining oxidation, adsorption, and coagulation was developed using the S(IV)–Fe(II) binary activated permanganate (PM) system, S(IV)–Fe(II)/PM. The efficacy of S(IV)–Fe(II)/PM pretreatment in mitigating UF membrane fouling was investigated for various raw water sources, including lakes, rivers, and seawater. The operational parameters of S(IV)–Fe(II)/PM pretreatment were optimized, and the underlying mechanisms for fouling alleviation were explored. Relative to conventional pretreatment methods, S(IV)–Fe(II)/PM pretreatment reduced reversible fouling-induced resistance by 13%–92% and irreversible fouling-induced resistance by 11%–86%. The S(IV)–Fe(II)/PM system exhibited optimal mitigation of membrane fouling at a PM:S(IV):Fe(II) dosage ratio of 2:3:3, with G rapid × T rapid = 45948, G slow × T slow = 12480, and a settling time of 30 min (where G is the velocity gradient and T is contact time). The effectiveness of S(IV)–Fe(II)/PM pretreatment in controlling UF membrane fouling can be attributed to the following mechanisms: 1) modification of feed water quality in terms of organic compound characteristics and concentration, colloidal particle quantity and size distribution, and microbial activity and quantity; and 2) adjustment of the membrane surface deposition environment, resulting in reduced polysaccharide and protein content, particle size distribution range, and biomass, as well as alterations in physicochemical properties such as hydrophilicity and interfacial free energy. This study highlights the efficacy of S(IV)–Fe(II)/PM pretreatment in ensuring high-quality UF effluent while effectively reducing membrane fouling, especially its potential for alleviating irreversible membrane fouling.
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