APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Fantao Kong,Yifan Huang,Meixin Chen,Ge Meng,Han Tian,Yafeng Chen,Ziwei Chang,Chang Chen,Wenping Sun,Xiangzhi Cui,Jianlin Shi
The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (Fe SA -N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N 4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N 4 moieties, the optimized Fe SA -N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials ( E 1/2 ) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using Fe SA -N/Cs-OAc as cathode delivers a power density of 165 mW cm −2 , and the maximum output power in H 2 -O 2 fuel cell reaches 640 mW cm −2 . The abundant mesoporosity makes most Fe-N 4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Aotian Gu,Peng Wang,Kaiwei Chen,Elvis Djam Miensah,Chunhui Gong,Yan Jiao,Ping Mao,Kai Chen,Jinlong Jiang,Ying Liu,Yi Yang
Based on two topologically distinct MOFs, the core–shell bimetallic MIL-101/ZIF-67 x (M/Z x ) were successfully prepared to activate the self-decomposition of peroxymonosulfate (PMS) for 2-chlorophenol (2-cp) degradation. The M/Z x not only inherited the merits of single-metal MOFs such as high surface area and pore volume, but also exhibited superior catalytic performance. In the M/Z x /PMS system, 90% of the 2-cp (100 mg/L) was removed within 10 min with a reaction rate of 0.241 min −1 . This observation was attributed to the synergistic catalysis of cobalt and iron active sites in M/Z x , which greatly promoted the Co 2+ /Co 3+ redox cycle, thereby enhancing the catalytic performance. Further investigation found that both radical and non-radical pathway jointly promote the degradation of 2-cp, and the singlet oxygen ( 1 O 2 ) mediated non-radical pathway serve a predominant role. Meanwhile, SO 4 ·- and · OH also accelerated this process. The possible degradation pathway was proposed by identifying the intermediates of 2-cp degradation. This work provides some new ideas for the design of multi-metal MOFs for environmental remediation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Nan Xue,Yue Zhang,Chunyan Wang,Xueyan Xue,Dandan Ouyang,Hui Zhu,Jiao Yin
Currently, it is a great challenge to improve the stability of Fe-based oxygen reduction reaction (ORR) catalysts in acidic medium, because the Fenton reaction between Fe-based catalyst and H 2 O 2 will reduce the stability of the catalyst. In this study, Fe, Cr and nitrogen-doped carbon (FeCr-N-C) was synthesized via co-impregnation of biomass walnut shells with metal precursor solutions. The FeCr-N-C catalyst has an onset potential of 0.88 V vs. RHE and outperforms the Fe-N-C catalyst in acidic media. Moreover, FeCr-N-C shows negligible activity decay (ΔE 1/2 = 14 mV) in 0.1 M HClO 4 after 20 000 cycles. The experimental results proved that the bimetal synergism can produce low yield of H 2 O 2 (<2%), which might attribute to variations of local electronic structure. The reactive oxygen species of the catalyst were analyzed by Ultraviolet-visible (UV-Vis) absorption spectra . It was proved that the presence of bimetal inhibited the Fenton reaction between Fe 2+ /Fe 3+ and H 2 O 2 , and further improved the stability of the catalysts. Hence, this study proposes an efficient strategy to facilitate the practical application of Fe-based catalysts in acidic media.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Chunfeng Shao,Lingmin Wu,Yinghua Wang,Konggang Qu,Hailiang Chu,Lixian Sun,Jianshan Ye,Baitao Li,Xiujun Wang
Single-atom Fe catalysts are a promising substitute to Pt catalysts for oxygen reduction reaction (ORR). Adjusting metal energy level through direct atomic interface regulation can effectively improve catalytic performance but still in its infancy. Herein, highly active nitrogen and sulfur dual-coordinated asymmetric Fe center anchored in carbon nanoparticles were developed. Spontaneously absorbed OH ligand is steadily anchored in asymmetric atomic interface, constructing new FeN 3 S-OH moiety. Theoretical calculations reveal that the incorporated S atom combined with OH ligand as energy level modifier effectively activate Fe center by electronic modulation and d -band center shift, rendering improved ORR activity of FeNSC-2Fe with E 1/2 of 0.913 V in alkaline, 0.806 V in acidic and 0.711 V in neutral media. The FeNSC-2Fe-based device displays high power density of 306 mW cm −2 in Zn-air battery and 2485 mW m −2 in microbial fuel cell . This work provides a new perspective for the controllable synthesis and performance optimization for electrocatalysts.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Meng Liu,Xiangzhe Yan,Lezhu Su,Hang Dong,Zhan Hu,Yuanqi Peng,Liqian Guan,Junjie Zhang,Zhi Zhou,Yongfa Zhu,Nan Zhou
Pyrolysis technology has been focused on waste plastics for recycling. However, there is rare research for reusing pyrolysis products (carbon nanotubes). Based on pyrolysis technology of waste polypropylene (PP) plastic, carbon nanotube coated Fe–Mo/MgO nanomaterial (CNT@Fe–Mo/MgO) was prepared by chemical vapor deposition to remove Gram-pathogenic bacteria. The addition of Mo and MgO promoted the cracking of PP plastic and the formation of MWCNTs. The as-obtained CNT@Fe–Mo/MgO can stimulate H 2 O/O 2 to produce abundant ·OH, ·O 2 − and 1 O 2 radicals, which probably resulting from the synergistic effect of delocalization of CNTs and REDOX pair of Fe 3 O 4 . Consequently, the removal rate of Escherichia coli and Staphylococcus aureus by CNT@Fe–Mo/MgO composite catalyst can reach 100% within 2h, without the help of any additional energy or active oxidant. At the same time, the material is remarkable stability and reusability with complete removal of pathogens after six cycles. This study not only provides a method for the synthesis of highly effective sterilizers , but also opens up a new direction for the application of functional carbon nanocomposites prepared by pyrolysis of waste plastics.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Bingzhe Jia,Huailin Yang,Lei Wang,Zhiqi Zhao,Xinming Wu
Compared with most transition metal based electrode materials, 2D M n+1 X n T x has high conductivity and good solvent compatibility. However, its low energy density hinders its application as supercapacitior electrode for electrochemical energy storage applications. Herein, the interface-pillared of Fe-MOF (MIL-100(Fe)) onto Ti 3 C 2 T x MXene layer, which provide rich electrochemical active sites, is achieved, and the MOF nanospheres with MXene nanosheets are subsequently converser into three dimensional multilayer porous nanostructures through the chemical bond couping. Therefore, the MOF nanospheres are anchored between the nansheets of MXene, enabling the fast ion transportation in the three dimensional nanostructures. Menanwhile, the MOF nanospheres prevent the aggregation of MXene nanosheets, and the laminar structure is maintained for more redox reaction sites within the hybrid electrodes through fast charge–discharge cycles. As a result, the MIL-100(Fe)/Ti 3 C 2 T x MXene electrode displays superior energy density (85.53 Wh kg −1 ), which is much higher than the other MXene-based electrodes as far as we know. This design strategy of 2D hybrid electrodes opens up a new way for the commercial application of high perfermance supercapacitor.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Zhenchao Lei,Ziyuan Huang,Yimin Lin,Yuwei Liu,Zhang Yan,Wenxiao Zheng,Huanxin Ma,Zhi Dang,Chunhua Feng
The corrosion of Fe(0) in the presence of O 2 in nature can lead to the oxidation of organic compounds, but the efficiency is very limited. Herein, attempts were made to establish a galvanic system that separates the anodic Fe(0) oxidation reaction and the cathodic O 2 reduction reaction using an air-breathing cathode. Compared with the chemical Fe(0)/O 2 system, it exhibited a substantially higher capability of destroying a variety of pollutants, such as organic dyes (12 types), phenol , nitrobenzene , acetaminophen, phenol, and ethylenediaminetetraacetic acid. The degradation rate constant of a model dye (i.e., Rhodamine B) increased from 0.047 min − 1 (chemical) to 1.412 min −1 (galvanic) under the passive air-breathing condition. The electric circuit design promoted Fe(0) dissolution to Fe(II) and triggered electron transfer that drives O 2 reduction to H 2 O 2 , two important species responsible for the generation of HO • at high abundance. In addition, the galvanic Fe(0)/O 2 system produces electricity while destroying pollutants. Tests with real Ni plating wastewater further demonstrated the capability of the system to oxidize complexed organics and phosphite. This study provides a new strategy for boosting the oxidative capacity of the Fe(0)/O 2 system, which shows promise for acid wastewater treatment .
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Ming Zhao,Shan Zhang,Jian Lin,Weihua Hu,Chang Ming Li
The high overpotential of oxygen evolution reaction (OER) is the main limitation of electrolytic water splitting efficiency for hydrogen production . Herein, Fe doped Ni 3 S 2 /MnS heterostructured nanosheets were grown on Ni foam (Fe-Ni 3 S 2 /MnS@NF) via a simple one-step solvothermal reaction. As-synthesized Fe-Ni 3 S 2 /MnS@NF exhibits excellent OER electrocatalytic activity in 1 M KOH, with an extremely low overpotential of 259 mV at 50 mA cm −2 as well as a small Tafel slope (39 mV dec −1 ), much better than Ni 3 S 2 -, Fe-doped Ni 3 S 2 -, and Ni 3 S 2 /MnS- nanosheets grown on NF. Results clearly reveal that the better electrocatalytic performance of Fe-Ni 3 S 2 /MnS@NF than its rivals is mainly due to the synergistic effect of Fe-doping and Ni 3 S 2 /MnS heterojunctions. In details, heterojunction combination with Fe-doping not only improves the conductivity of catalysts but also modulates the electronic configuration of active sites and optimizes the adsorption capacity of oxygen-containing intermediates, thus achieving rapid reaction kinetics and high electrocatalytic performance. This work provides insights into the synergistic regulation of electrocatalytic activity of non-noble catalysts toward high efficiency energy conversion.
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CARBON
·
2021
·
IF 9.594
Yu Ma,Ding Chen,Dongdong Zhang,Hao Yu,Yapeng Zheng,Weijun Li,Lin Wang,Qiao Liu,Weiyou Yang
Freestanding air cathode catalyst with exceptional catalytic bifunctions for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is highly desirable for exploring rechargeable Zn–air batteries (ZABs) with low cost and high reliability. Here, a facile and scalable approach is demonstrated to prepare efficient and robust freestanding cathode catalyst that consists of dispersed Fe 3 C nanoparticles , rich Fe-N x /N-C species and carbon fibers networks with large specific surface area, which is based on one-pot in-situ coupling of Fe and N induced active sites within bacterial cellulose-derived carbon fibers networks. Its bifunctional activity parameter (Δ E ) for ORR and OER is 0.79 V, superior to those of single Fe- or N- modulated counterparts, and comparable to the state-of-the-art Pt/C + RuO 2 catalyst (0.79 V). This material can be directly used as freestanding and binder-free catalyst layer , and as-assembled ZABs exhibit a larger peak power density (173 mW cm −2 ), higher specific capacity (717 mA h g −1 , 10 mA cm −2 ) and better cycle stability (negligible activity decay after 165 h charge/discharge cycles) than those of Pt/C + RuO 2 -based devices, representing their potential applications in advanced energy conversion systems.
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ACS ES&T Engineering
·
2021
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IF 0
Ying Liu,Yulin Yang,Wei Miao,Ningjie Du,Dandan Wang,Hehe Qin,Shun Mao,Kostya Ken Ostrikov
Electro-Fenton (EF) is one of the promising clean and renewable technologies for organic pollutant control. However, insufficient hydrogen peroxide (H2O2) generation and the subsequent hydroxyl radicals (•OH) conversion still prevent the wide applications of EF. Herein, we report a Ce-doped vertically aligned α-FeOOH nanoflakes anchored on a carbon felt (CF) cathode for EF operation. In this system, a high concentration H2O2 (113.6 mg/L on 4 cm2 cathode) is generated in 60 min, and being efficiently catalyzed to •OH by virtue of the active nanoedge (1.6 nm thickness) of Ce-doped α-FeOOH. The •OH production rate is calculated as high as 4.2 mM/W/cm2/min, which is ∼6.6-fold higher compared with the unmodified CF electrode. Moreover, this novel cathode achieves a complete removal (100% removal rate) of ultrahigh concentration chloramphenicol (1.1 mM, 355 mg/L) in 8 h and a high mineralization rate (94%) in 29 h in a scaled-up EF system. Density functional theory calculations (DFT) reveal that the Ce doping in α-FeOOH greatly promotes the conversion of H2O2 into •OH. This study not only offers a novel cathode structure for EF process but also opens radically new prospects for applied environmental catalysis.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ping-An Yang,Yuxuan Huang,Rui Li,Xin Huang,Haibo Ruan,Mengjie Shou,Wanjun Li,Yuxin Zhang,Nan Li,Lichao Dong
Ag-coated Fe (Fe@Ag) core–shell nanowires (NWs) with enhanced electromagnetic wave absorption were successfully synthesized by the liquid-phase reduction method and the layer-plus-island growth mode. Changing the molar ratio of Fe to Ag controlled the Ag shell thickness to produce different impedance matching and attenuation constants of the Fe@Ag core–shell NWs. The Fe@Ag core–shell NWs with a Fe:Ag ratio of 2:1 significantly improved optimal microwave absorption performance as compared to raw Fe NWs. At a mass fraction of 25%, the minimum reflection loss (RL min ) can reach − 58.69 dB at 7.53 GHz with a matching absorber thickness of 3.36 mm. In addition, the effective absorption bandwidth (EAB, RL ≤ − 10 dB) can be extended to 7.32 GHz, to cover the majority of the C and X bands. Three major aspects contribute to the superior microwave absorption performance: the complementary effect of the polarization of Fe-Ag interface, the impedance matching improvement stems from a proper eddy current, and the small-scale effect caused by a one-dimensional structure. This study demonstrates the promising high-efficiency microwave absorbing capabilities of Fe@Ag core–shell NWs for future use in practical applications.
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ANALYST
·
2021
·Vol. 146
·期 20
·6187-6192
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IF 4.616
Guihua Zhang,Xinyi Zou,Hua Li,Yi He
Triacetone triperoxide (TATP) explosives, a popular choice for terrorists, have been used in many violent terrorist attacks all over the world. However, simple, rapid, and on-site detection methods of TATP are still lacking. Herein, we present a visual colorimetric method for on-site and rapid detection of TATP based on a Fe(II)-promoted thermal decomposition process of TATP. We discovered that TATP can be decomposed into H2O2 under heating conditions, and it reacts with Fe2+ to produce hydroxyl radicals (˙OH) and Fe3+via the Fenton reaction. The resulting ˙OH and Fe3+ further oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to a yellow oxidized product (oxTMB). These reaction processes remarkably promote the chemical equilibrium shift and decrease the activation energy. Using the TATP-Fe2+-TMB ternary chromogenic system, the present colorimetric assay for TATP shows a dynamic range of 0.5–30 μM with a low detection limit of 0.12 μM. Additionally, common substances (e.g., inorganic salts, small organic substances, and polymers) do not interfere with TATP detection. This assay can be used for analyzing TATP in real water and camouflage samples. Furthermore, a test-paper-based method was also successfully developed for visual, rapid and on-site detection of TATP.
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