ENERGY & FUELS
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2021
·
IF 3.605
Jianwen Guo,Jiang Wu,Yu Guan,Jianmin Wang,Qizhen Liu,Xu Mao,Xuemei Qi,Ping He,Huaning Wang
A Z-scheme heterojunction polyhedral-shaped BiOIO3/MIL-53(Fe) photocatalyst is prepared by a solvothermal method. The samples are characterized by XRD, XPS, SEM, TEM, FT-IR, UV–vis, PL, and other material characterization analysis methods. The photocatalytic performance of photocatalysts is studied for removal of vapor-phase mercury (Hg0) under visible-light irradiation. The results suggest that the Hg0 removal efficiency of the BiOIO3/MIL-53(Fe) composite is significantly improved compared with that of MIL-53(Fe). When the molar ratio of BiOIO3 and MIL-53(Fe) is 2:1, the BiOIO3/MIL-53(Fe) composite photocatalyst exhibits the best Hg0 removal efficiency, reaching 74.19%. BiOIO3 and MIL-53(Fe) form a Z-scheme heterojunction with a suitable energy band structure, which results in the effective separation of photoinduced electron–hole pairs and delays their recombination. Finally, the photocatalytic oxidation mechanism of Hg0 by the BiOIO3/MIL-53(Fe) composite is proposed, which paves the way for the study of the built-in electric field and electron transport channels between binary photocatalyst materials.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 3
·034516
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IF 4.316
Kai Li,Yafeng Jin,Wenming Gao,Shoucai Xue,Ming Zhang
A critical issue for massive production of metal-supported solid oxide fuel cell is cathode processing due to the contradicting of the metal support and the cathode with regard to the sintering atmosphere. Herein, LSM-BSCF (La0.8Sr0.2MnO3-δ coated Ba0.5Sr0.5Co0.8Fe0.2O3-δ) cathodes on Ni-Fe alloys supported SOFCs (NF-SOFCs) are fabricated by an ex situ sintering approach and electrochemical evaluation in humidified H2 fuel. The ex situ sintering of cathodes on NF-SOFCs are performed at 1050 °C in air with metal oxide support consisted of NiO and 10 at% Fe2O3, and then the oxide support is reduced in situ into Ni-Fe alloys during testing. Cross-section microstructure analysis shows clear evidence that each layer is well adhered to each other after reduction and the suitable microstructure of ex situ sintered cathode is observed after sintering at 1050 °C. In the single-cell test, a higher peak power density is achieved for NF-SOFC with ex situ sintered LSM-BSCF in comparison with in situ sintered cells, revealing a beneficial effect of ex situ sintered cathode on cell performance. The durability measurement and post-test analysis confirm the sufficient adherence and mechanical stability between ex situ sintered LSM-BSCF cathode and GDC (Ce0.9Gd0.1O1.95) electrolyte. The successful electrochemical characterizations of NF-SOFCs with ex situ sintered LSM-BSCF cathode confirm the applicability of the novel sintering procedure.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xixi Chen,Shujuan Zhan,Dingsheng Chen,Chun He,Shuanghong Tian,Ya Xiong
Grey Fe doped CeO 2-σ with tunable surface and bulk oxygen vacancies (OVs) were facilely prepared by a hydrothermal method. The light absorption, charge transfer efficiency, and catalytic activity and mechanism closely depended on the OVs. By tailoring the surface and bulk OVs, the catalytic activity of grey ceria was boosted due to the enhanced production of reactive oxygen species (i.e. OH, surface O). Density functional theory calculations show that the OVs, especially the bulk OVs, modulate the electronic structure for narrowing the bandgap and accelerating the charge transfer. Meanwhile, the surface OVs more promote the adsorption of ozone and the bulk OVs more induces the dissociation of ozone into reactive surface O. The calculation results agree well with the experimental observations. This study provides a simple method for engineering the surface and bulk OVs of ceria and gains insight into their roles in photocatalytic ozonation .
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Liuyang He,Lixin Lv,Suresh C. Pillai,Hailong Wang,Jianming Xue,Yongfei Ma,Yanli Liu,Yulin Chen,Li Wu,Zulin Zhang,Lie Yang
Iron/copper bimetallic nanoparticles based sludge biochar (Fe/Cu-SBC) was prepared by using a modified co-precipitation route. The Fe/Cu-SBC system prepared was subsequently applied to activate periodate (IO 4 − ) to degrade diclofenac sodium (DCF) by using UV light at room temperature (25 °C). The physicochemical properties of both SBC and Fe/Cu-SBC such as morphology, physical properties, crystal structures and functional groups were examined. The type and number of surface functional groups were found to be increased and the catalytic performance was improved by the modification of Fe/Cu bimetallic nanoparticles. The influence of various parameters to evaluate the catalytic efficiency such as periodate (PI) concentration, dosage of catalysts, UV power, initial pH and coexisting anions were investigated. Under the optimized conditions (pH 6.9, UV-power 60 W, PI concentration of 5 mM and 0.1 g Fe/Cu-SBC), it was observed that 99.7% of DCF was degraded with a pseudo-first-order kinetics reaction constant 9.39 × 10 −2 min −1 . The radical scavenging experiments showed that IO 3 radicals were the predominantly reactive oxidants in the Fe/Cu-SBC/UV system. Therefore, this investigation provides a feasible alternative for the degradation of PPCPs in wastewater.
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高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Jinbin Lin,Jing Zou,Hengyu Cai,Yixin Huang,Jiawen Li,Junyang Xiao,Baoling Yuan,Jun Ma
In this study, a commonly used reducing agent, hydroxylamine (HA), was introduced into Fe(II)/PAA process to improve its oxidation capacity. The HA/Fe(II)/PAA process possessed high oxidation performance for diclofenac degradation even with trace Fe(II) dosage (i.e., 1 μM) at pH of 3.0 to 6.0. Based on electron paramagnetic resonance technology, methyl phenyl sulfoxide (PMSO)-based probe experiments and alcohol quenching experiments, Fe IV O 2+ and carbon-centered radicals (R-O • ) were considered as the primary reactive species responsible for diclofenac elimination. HA accelerated the redox cycle of Fe(III)/Fe(II) and itself was gradually decomposed to N 2 , N 2 O, NO 2 − and NO 3 − , and the environmentally friendly gas of N 2 was considered as the major decomposition product of HA. Four possible degradation pathways of diclofenac were proposed based on seven detected intermediate products. Both elevated dosages of Fe(II) and PAA promoted diclofenac removal. Cl − , HCO 3 − and SO 4 2− had negligible impacts on diclofenac degradation, while humic acid exhibited an inhibitory effect. The oxidation capacity of HA/Fe(II)/PAA process in natural water matrices and its application to degrade various micropollutants were also investigated. This study proposed a promising strategy for improving the Fe(II)/PAA process and highlighted its potential application in water treatment.
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ACS Catalysis
·
2021
·
IF 13.084
Ting Wang,Yuebing Xu,Yufeng Li,Lei Xin,Bing Liu,Feng Jiang,Xiaohao Liu
Conversion of syngas into aromatics via the Fischer–Tropsch (FT) route provides a promising way to supply the value-added chemicals. However, it is still a great challenge to achieve controllable aromatics selectivity with good stability. Herein, we report the Na-mediated bimetallic Fe–Ni catalyst simply particle mixed with HZSM-5, which can boost the stable and selective production of aromatics from the syngas. In detail, FeNiOx(5:1)-0.41Na exhibits quite stable catalytic activity with notably higher selectivity to light α-olefins (C2=–C4=) compared to α-Fe2O3-0.75Na. Various characterizations suggest that an appropriate addition of Ni with Na substantially regulates iron carbide formation and suppresses carbon deposition owing to the electron donation of Fe to Ni reducing CO adsorption and dissociation. Interestingly, extra Na results in remarkably increased selectivity to C1o–C4o, despite the fact that Na shows the ability to suppress hydrogenation. Both characterizations and density functional theory (DFT) calculations demonstrate that the addition of Na weakens the Fe–Ni interaction and reduces electron transfer from Fe to Ni, which promotes C1o–C4o formation as Ni tends to reflect its intrinsic catalysis. DFT calculations confirm that the adsorbed CH2 species at the Ni–Fe interface prefers to undergo coupling to form C2H4, and the formed C2H4 spontaneously desorbs from the surface, indicating that the formation of lower olefins is favorable and further chain growth is inhibited. This could be attributed to the fact that the accumulated electron at the Ni–Fe interface weakens the binding strength of CH2 and C2H4 species because of electronic repulsion. Furthermore, the effects of FT product distribution on aromatics formation were also investigated. FeMnOx(5:1)-0.40Na produces longer olefin-rich hydrocarbons in C5+ owing to oxygen vacancy-assisted CO dissociation, leading to highly branched monocyclic aromatics and faster HZSM-5 deactivation because of increased coking from the isomerization–hydrocracking of long hydrocarbons. In contrast, FeNiOx(5:1)-0.41Na-HZSM-5 produces major light aromatics about 65.7% including toluene, ethyl-benzene, and xylene in total aromatics with about 98.6% aromatics in the liquid phase, which benefits from the fact that FeNiOx(5:1)-0.41Na makes shorter hydrocarbons in C5+ and/or Ni metal has a strong ability of H2 dissociation to provide atomic H spillover onto HZSM-5. Thus, HZSM-5 also shows improved stability. Note that the mixed catalysts with a high Na content indicate a substantial Na+ migration to increase light α-olefins in the gas phase owing to suppress H-transfer reaction. This study provides deep insights into how to develop stable and selective iron-based catalysts for the production of FT products and its further conversion into value-added light aromatics.
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Biomaterials Science
·
2021
·Vol. 9
·期 20
·6772-6786
·
IF 6.843
Sulan Luo,Yiting Zhao,Kewei Pan,Yixian Zhou,Guilan Quan,Xinguo Wen,Xin Pan,Chuanbin Wu
The low oxygen level in tumors significantly reduces the antitumor efficacy of photodynamic therapy (PDT). The provision of O2 and monomeric hydrophobic photosensitizers (PSs) under physiological conditions would greatly help to shrink malignant tumors. We take advantage of the high porosity and multifunctionality of metal–organic frameworks (MOFs) to fabricate a simple all-in-one nanoplatform mediated by microneedle delivery to achieve synergistic O2 evolution and chemophototherapy. An iron(III)-based MOF (MIL-100(Fe)) acted not only as a vehicle for the concurrent delivery of zinc phthalocyanine (ZnPc) and doxorubicin hydrochloride (Dox), but also to supply O2 by decomposing hydrogen peroxide (H2O2) in the tumor microenvironment via a Fenton-like reaction. In vitro and in vivo experiments indicated that the nanoplatform had excellent biocompatibility and exerted enhanced anticancer effects. The encapsulated drug was sustainably released from the nanoplatform skeleton in response to acidic tumor microenvironments. Moreover, upon 660 nm light irradiation, ZnPc effectively produced reactive oxygen species (ROS) due to the reduction of hypoxia by MIL-100(Fe). A microneedle technique was adopted to directly deliver the nanoplatform into superficial tumors rather than via systemic circulation. Hence, this study provides a new strategy for more efficient chemophototherapy of hypoxic superficial tumors.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Haiyuan Chi,Chengjun Li,Mei Huang,Jinquan Wan,Xiaoxia Zhou,Bing Yan
Sulfate radicals-based advanced oxidation processes are regarded as effective methods for removing organic contaminants. However, current removal technologies are often unable to achieve satisfactory results due to the low concentrations and high stability that are frequently characteristics for many types of organic contaminants. To improve the efficacy of using sulfate radicals to remove organic contaminants, we designed metal–organic frameworks (Fe(II)-MOFs) modified with enrichment and specific recognition of molecular imprinting layer (Fe(II)-MOFs@MIP). Using dibutyl phthalate (DBP) as the model target contaminant, the selectivity coefficient towards DBP was 7.28 for adsorption and 4.46 for catalytic degradation of Fe(II)-MOFs@MIP, which is excellent for most of the imprinted material. Additionally, we achieved the accurate recognition (169.25 μg × g −1 ) and efficient degradation (0.071 min −1 ) of DBP reducing levels to 100 μg × L -1 . UV–vis analysis confirmed that specific recognition of DBP was mainly through hydrogen bonding and π-π interaction, while in-situ Raman and radical quenching experiments showed that the imprinting layer could accurately adsorb and produce the spatial confinement effects on target contaminants, thereby reducing the transfer distance of free radicals. As a result, we show that Fe(II)-MOFs@MIP can achieve efficient targeted degradation of DBP, opening up a new avenue for the removal of this and other highly stable organic contaminants present at low concentrations in environmental systems.
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高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2021
·
IF 2.475
Xuekai Zhang,Kanggen Zhou,Qingyuan Lei,Yan Xing,Changhong Peng,Wei Chen
A new approach was developed using NaH2PO4 as the stripping agent for Fe stripping from Fe-loaded Aliquat 336 during rare-earth elements recovery from red mud leachate. Owing to the strong coordination between Fe3+ and H2PO4‒, Fe mainly exists as FeH2PO42+ at [H2PO4‒] higher than 0.5 M, which can be readily stripped. The results showed a maximum Fe stripping efficiency of 95.5% under optimal condition. Moreover, the extraction capacity of the extractant after stripping was comparable to that of fresh extractant, and decreased only by 2% after 6 cycles, indicating the robustness of this approach for Fe stripping and extractant regeneration.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Wanliang Yang,Meng Chen,Jiayuan Zhou,Yingnan Duan,Yinmin An,Mao Liu,Mengkui Tian
Porous carriers play an important role in the catalytic transformation of syngas into higher alcohols, which promises higher sustainability in C1 chemistry. In this work, a series of hierarchical hollow silica spheres (HHSS) supported Cu-Fe bimetal catalysts were successfully prepared through ultrasonic-assisted impregnation for higher alcohols synthesis from syngas. Structural characterization results indicate that the hierarchical hollow structure of HHSS support can be maintained and the Cu-Fe bimetallic nanoparticles are highly dispersed on HHSS surface. The catalytic performances of samples in the test of CO hydrogenation for higher alcohols synthesis were investigated. The results revealed that the conversion rate of CO and the selectivity of C 2+ OH alcohol increased first and then decreased with the decrease of the amount of Cu content in the Cu x Fe y @HHSS catalyst. The highest CO conversion, alcohol selectivity and STY ROH over Cu-Fe@HHSS catalyst are 65.1 %, 46.6 %, and 118.1 gkg −1 h −1 , respectively. It was found that a large number of CuFe 2 O 4 were formed in Cu-Fe@HHSS catalyst and also confirmed that the CuFe 2 O 4 spinel and CuO-CuFe 2 O 4 were converted to Cu-Fe 5 C 2 composite in the spent Cu-Fe@HHSS catalyst, which can enhance the synergy between Cu-Fe bimetals. Furthermore, copper and iron are highly dispersed on HHSS after the reaction, which enhances the structural stability of the catalyst. Based on the development and utilization of low-cost catalysts and the production of clean liquid fuels, HHSS has a great prospect of catalyst support in the energy field.
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ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Yun Bai,Doudou Wu,Wei Wang,Pei Chen,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, the application of organic acids as chelating agent , including citric acid (CA), tartaric acid (TA), oxalic acid (OA) and ethylenediaminetetraacetic acid (EDTA), to enhance the degradation performance of MgO 2 /Fe(III) system was investigated in the terms of chelating agent dosage, Fe(III) dosage, reaction temperature, initial solution pH and inorganic anion. When the molar ratio of MgO 2 /Fe(III)/chelating agent was 1 : 0.7 : 0.3, the degradation efficiencies of Rhodamine B (RhB) increased from 6.7% (without chelating agent) to 42.3%, 98.5%, 48.9% and 25.8% within 30 min for CA, TA, OA, and EDTA, respectively. The promotion effect was mainly attributed to the chelation between chelating agents and Fe(III), rather than the acidification of chelating agents. The pseudo-first-order kinetic model well fitted RhB degradation in MgO 2 /Fe(III)/TA system, and the kinetic rate constant reached up to 0.295 min −1 . Hydroxyl radical was confirmed to be the dominant active species to degrade organics in the MgO 2 /Fe(III)/TA system. Notably, the degradation system could work in a broad pH (3–11) and temperature (5–35 °C) range. Moreover, the MgO 2 /Fe(III)/TA system can also effectively degrade methylene blue , tetracycline and bisphenol A. This work provided a new, efficient and environmentally-friendly Fenton-like system for stubborn contaminant treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Wei Zhang,Wei Liu,Guoliang Li,Wei Du,Jianbo Lu,Jianguo Song,Qixia Yang,Xiangming Li,Huizhong Xu,Xu He,Jun Ma
The para arsanilic acid ( p -ASA) used as feed additive in the poultry and swine industries tends to transform into more toxic inorganic arsenic (As(V) and As(III)), leading to a greater risk to human health and environmental system. In this study, simultaneous adsorption and oxidation of p -ASA was achieved by a synthesized highly efficient nanostructured Fe-Ti-Mn composite oxide (FTMO), with a high specific surface area of 424.7 m 2 /g. The maximum adsorption capacity for p -ASA could be as high as 45.6 mg/g, meanwhile the combined oxidation/photo-oxidation processes led to the formation of intermediate containing hydrazine group, however, without release of toxic inorganic As(III) and As(V). The p -ASA adsorption by FTMO was verified as the chemisorption process with the formation of inner-sphere complexes at the solid/water interface, which was prominently influenced by solution pH, coexisting ions and humic acid, however relatively insensitive to ionic strength. The systematic characterization by FTIR, XPS, EPR and XANES revealed that Fe phase of FTMO played the dominant role for p -ASA adsorption, while Mn and Ti phases were responsible for the oxidation and photo-oxidation of p -ASA, respectively.
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