PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
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IF 7.926
Chunying Dong,Yuang Pang,Yan Chen,Zhan Gao,Meiqiang Cai,Micong Jin,Zongsu Wei
Sludge based catalysts (SBCs) has been considered as a promising and viable approach to sludge reclamation. Herein, we fabricated bimetallic Fe-Ti doped SBCs via a facile synthesis with sludge containing polyacrylamide (PAM) as N-precursor. The adsorption capacity and degradation efficiency of as-synthesized SBCs were assessed using tetracycline (TC) as a target pollutant, in which PAM in sludge played a dual role by promoting porosity, active sites, and structural defects beneficial for persulfate (PS) activation. Fe-Ti doping induced the activation of PS by a fast redox cycle of Fe 3+ /Fe 2+ associated with the coexistence of Ti 4+ /Ti 3+ , which enabled an efficient electron transfer between the catalyst and PS. The synergistic effect of PAM-derived N doping and Fe-Ti bimetals resulted in prevention of iron leaching and enhanced catalyst stability over a wide pH range. The surface SO 4 •− was the primary oxidant in the TC degradation process based on free-radical quenching experiments, and degradation pathways of TC were proposed given the intermediate evidence from UPLC-HRMS analysis. This study promotes the reclamation of PAM-containing sludge providing an eco-friendly and efficient process to activate PS for wastewater treatments .
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Fenli Liu,Yujing Ren,Jianglin Duan,Pengcheng Deng,Jianyu Lu,Huibin Ge,Xin Liu,Qixing Xia,Haifeng Qi,Na Yang,Yong Qin
Activating hydrogen peroxide (H 2 O 2 ) to produce hydroxyl radical ( • OH) (Fenton-like process) is of great importance in heterogeneous catalytic oxidations. However, most of transition metal nano-catalysts as well as recently reported carbon supported Fe-N 4 single atom catalysts (SACs) suffer from unsatisfactory catalytic performance. Herein, a novel Fe 1 /C 3 N 4 SAC with Fe-N 5 active site was constructed. Using this SAC, the electron/structure-symmetry of Fe-N 4 site can be broken by axial nitrogen-coordination, which transforms less active Fe-N 4 species into highly active Fe-N 5 species in Fenton-like reaction. Specifically, Fe-N 5 site exhibits an unprecedented activity for 3,3′,5,5′-tetramethylbenzidine oxidation, which is at least one order of magnitude more active than reported Fe-N 4 /C SACs. Mechanism studies reveal that the unique role of axial nitrogen-coordination over Fe-N x sites is to change the adsorption behavior of H 2 O over Fe-N 5 site without influencing H 2 O 2 activation. This discovery provides a new approach for rationally designing efficient catalysts in Fenton-like reactions.
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CHEMOSPHERE
·
2022
·
IF 8.943
Jiaojiao Yang,Binyu Guo,Lei Li,Quanyuan Chen,Chensi Shen,Juan Zhou
The limited regeneration of Fe 2+ in the Fe-catalyzed advanced oxidation processes (AOPs) constrained its application for the removal of organic pollutants. Herein, MoSe 2 was introduced to promote the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in the Fe 2+ /PMS system. Compared with Fe 2+ /PMS processes, the 2,4-D degradation efficiency and PMS decomposition rate respectively increased by 73.8% and 84.2% in the MoSe 2 /Fe 2+ /PMS system. DFT simulation results suggested that Se atoms acted smoothly as the bridge supporting the charge transfer from Mo to adjacent Fe atoms, which led to the reduction of Fe 3+ . The rapid regeneration of Fe 2+ boosted the activation of PMS and the degradation of pollutants. Additionally, the electron paramagnetic resonance (EPR) and quenching experiments results indicated that SO 4 ∙ − , ∙OH, and 1 O 2 accounted for 2,4-D degradation, and SO 4 ∙ − and 1 O 2 predominated the reaction. The Mo based co-catalysts showed better co-catalytic effect than the W counterparts, and the moderate adsorption for PMS and lower electron transfer electron transfer resistance accounted for the more excellent co-catalytic performance of MoSe 2 than that of WSe 2 . In addition, the degradation efficiency of 2,4-D was up to 95.5% after five cycles of MoSe 2 in the co-catalytic system. The coexistent humic acid (HA) and Cl − showed ignorant negative effect on the degradation, while HCO 3 − would depress the oxidation reaction. The acidic etching wastewater can be applied as the Fe ions source in this co-catalytic process to remove 2,4-D effectively.
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PubMed
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Weiwen Wang,Jianing Qu,Chaojie Li,Lexin Guo,Xianxin Fang,Guanghui Chen,Jihai Duan
Biomimetic photocatalytic nitrogen fixation is considered as a potential alternative to the Haber-Bosch method, which is an ideal pathway for nitrogen reduction. The development of efficient bionanocatalysts is a serious challenge in the current field of biomimetic nitrogen fixation. Here, we introduced a second metal in the MIL-88A/Fe mesh by metal doping to build a Mo-doped MIL-88A(Fe/Mo)/Fe mesh biomimetic system. The catalyst is a rod-like structure synthesized in situ by hydrothermal method using iron mesh as the substrate, and its rough surface is favorable for the adsorption of N 2 . The introduction of Mo provides a two-electron transfer pathway for the reaction, and the formation of the "MoFe cofactor" effectively promotes charge separation and inhibits the photoelectron-hole complexation. In addition, we kept the catalyst above the liquid surface and provided the proton source through water vapor, which solved the problem of the low solubility of N 2 in water and poor mass transfer efficiency. The results show that the biomimetic photocatalyst has good photoresponsiveness in the whole visible region, and the synergistic effect between the two metals makes the MIL-88A (Fe/Mo 0.017 )/Fe mesh exhibit better photocatalytic performance, and its nitrogen fixation efficiency reaches about 9.6 times that of the original MIL-88A/Fe mesh. This study provides a new idea for the design of photocatalytic ammonia biomimetic photocatalysts.
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高影响因子
ADVANCED MATERIALS
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2022
·Vol. 35
·期 5
·2208034
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IF 32.086
Kai Jia,Jun Ma,Junxiong Wang,Zheng Liang,Guanjun Ji,Zhihong Piao,Runhua Gao,Yanfei Zhu,Zhaofeng Zhuang,Guangmin Zhou,Hui-Ming Cheng
A large amount of spent LiFePO 4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li + diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li + migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d-band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen-doped carbon. The Fe O bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d-band center. The Li + diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.
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高影响因子
Journal of Cleaner Production
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2022
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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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JOURNAL OF HAZARDOUS MATERIALS
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2022
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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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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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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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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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高影响因子
ELECTROCHIMICA ACTA
·
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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APPLIED SURFACE SCIENCE
·
2022
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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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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