INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Qiulin Li,Xiang Li,Ke Zhang,Jiaqi He,Yongbing Lou,Jinxi Chen
There is an urgent need to design effective and affordable noble metal-free oxygen evolution electrocatalysts for the realization of hydrogen production technology through overall water splitting. In this work, we synthesized CoMoO 4 /Fe-MOF composite catalysts on nickel foam by solvothermal method and explored them as electrodes towards oxygen evolution reaction. At 10 mA cm −2 , CoMoO 4 /Fe-MOF demonstrated a small overpotential of 238 mV, with a relatively small Tafel slope of 49.22 mV dec -1 and exhibited excellent stability after 30 h of testing. The enhanced OER activity and good durability of CoMoO 4 /Fe-MOF could be attributed to the self-supported growth of Fe-MOF nanosheets as well as the tight binding to the rod-like CoMoO 4 . The coupling of CoMoO 4 with Fe-MOF established a rich boundary, thus improving conductivity, increasing specific surface area and exposing more active sites. These results suggested that the combination of MOFs with binary transition metal oxides provided an effective route to develop robust and efficient electrocatalysts.
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Catalysts
·
2023
·Vol. 13
·期 6
·948
·
IF 3.9
Rui Hu,Tianye Wang,Yifan Wang,Yuan Zhu,Li Xie,Enhui Xing,Yu Wu,Zhijian Da
A nano-hollow zeolite-encapsulating ultra-fine Fe nanoparticle catalyst denoted as Fe@n-hS-HT was successfully synthesized through a simple water steam treatment of the Fe@n-hS catalyst prepared by the “dissolution–recrystallization” (D-R) method. The Fe@n-hS-HT catalyst had a hierarchical porous structure and a high dispersion of Fe2O3particles with a size of 3.4 nm. Furthermore, the results of several characterization methods, such as XRD, HAADF-STEM, and H2-TPR, further demonstrated the transformation of the skeleton Fe in Fe@n-hS into Fe2O3, which was uniformly dispersed in the Fe@n-hS-HT catalyst. Meanwhile, Fe@n-hS-HT had significantly higher selectivity and yield of C2-C4=than the reference catalysts Fe/S and Fe@n-hS, which provided strong proof for the confined catalysis of the metal@zeolite catalyst.Keywords:hollow zeolite;Fischer–Tropsch synthesis;encapsulation;iron catalyst
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 15
·1-12
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IF 2.8
Pan Yusong,Zhu Yuan,Wang Yuanqing,Huang Run,Pan Chengling
Based on the strong capability of transition metal ions for peroxymonosulfate (PMS) activation and highly affinity of MoS 2 towards PMS, thus decorating MoS 2 with transition metal ions would efficiently activate PMS for degradation of organic pollutants. In this work, Co/Fe co-doped MoS 2 catalyst were synthesized by simple chemical method. The prepared Co/Fe co-doped MoS 2 catalyst displayed excellent catalytic activity for organic pollutant degradation. The removal efficiency of RhB and MB is 99% in 6 min and 98% in 15 min under PMS system, respectively. Both the capture experiment and EPR results verified that 1 O 2 played an important role in the organic pollutant degradation process in PMS system. The catalytic mechanism revealed that the synergistic effect between Mo ion and Co/Fe ions is beneficial for boosting the catalytic properties of Co/Fe co-doped MoS 2 catalyst. The cycle experiments confirmed that Co/Fe co-doped MoS 2 possesses excellent chemical stability and re-usability.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 33
·80279-80292
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IF 5.8
Zhang Yaping,Zhang Duoxin,He Yufeng,Wang Zeyuan,Song Pengfei,Wang Rongmin
The environment and human health are in danger due to the long-term enrichment and buildup of organic pesticides, dyes, and harmful microbes in wastewater. The development of functional materials that are efficient for treating wastewater remains a significant problem. Eco-friendly hexagonal spindle-shaped Fe-MOFs (Hs-FeMOFs) were created in this study under the influence of cationic copolymer (PMSt). The mechanism of crystal growth and development of its unique morphology were described after looking into impact factors for the ideal circumstances and being characterized by XRD, TEM, XPS, and other techniques. It revealed that Hs-FeMOFs possess an enormous supply of adsorption active sites, a strong electropositivity, and the nanometer tip. Then, typical organic pollutants, such as herbicides and mixed dyes, as well as biological pollutants bacteria, were chosen to assess its efficacy in wastewater treatment. It was discovered that the pendimethalin could be quickly removed in wastewater and the removal rate reached 100% within 10 min. In separation of mixed dyes, the retention rate of malachite green (MG) reached 92.3% in 5 min and with a minimum inhibitory concentration of 0.8 mg/mL and demonstrated strong activity due to the presence of cationic copolymers. In actual water matrix, Hs-FeMOF could also play excellent adsorption and antibacterial activity. In summary, a novel, environmentally friendly MOF material with good activity was successfully created by cationic copolymer induction. It offers a fresh approach to develop functional materials in wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chengyu Huangfu,Shuning Yu,Bo Tong,Anni Yang,Jiafei Lyu,Xianghai Guo
MIL-100(Fe) is a kind of metal–organic frameworks (MOFs) with robust water and chemical stability. The adsorption kinetics, isotherms, thermodynamics and regeneration of MIL-100(Fe) were investigated to illustrate the process of efficient lithium adsorption. The adsorption kinetics of MIL-100(Fe) followed Pseudo-second-order model, and the lithium adsorption equilibrium was reached rapidly in 2 h. Langmuir model fit best with the adsorption isotherms, indicating chemisorption of lithium ions on MIL-100(Fe) and possibly a monolayer adsorption process. By calculating thermodynamic parameters (Δ G θ , Δ H θ and Δ S θ ), the adsorption of lithium on MIL-100(Fe) can be illustrated by a spontaneous endothermic process. The adsorption mechanism involved electrostatic interaction, impact of crystal defect sites and coordinative interactions between metal active sites and lithium ions (Fe—F‧‧‧Li). MIL-100(Fe) was regenerated for four cycles, and there was only a slightly decrease in adsorption capacity and the morphology remained stable. Combined with extremely short equilibrium time and high stability, MIL-100(Fe) can be a promising adsorbent for lithium extraction.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 25
·e2301011120
·
IF 11.1
Fa Yang,Ping Song,Xin Ge,Yan Wang,Takao Gunji,Wei Zhang,Xiao Zhao,Weilin Xu
As a sustainable approach for N2 fixation, electrocatalytic N2 reduction reaction (N2RR) to produce ammonia (NH3) is highly desirable with a precise understanding to the structure-activity relationship of electrocatalysts. Here, firstly, we obtain a novel carbon-supported oxygen-coordinated single-Fe-atom catalyst for highly efficient production of ammonia from electrocatalytic N2RR. Based on such new type of N2RR electrocatalyst, by combining operando X-ray absorption spectra (XAS) with density function theory calculation, we reveal significantly that the as-prepared active coordination structure undergoes a potential-driven two-step restructuring, firstly from FeSAO4(OH)1a to FeSAO4(OH)1a′(OH)1b with the adsorption of another –OH on FeSA at open-circuit potential (OCP) of 0.58 VRHE, and subsequently restructuring from FeSAO4(OH)1a′(OH)1b to FeSAO3(OH)1a″ due to the breaking of one Fe-O bond and the dissociation of one –OH at working potentials for final electrocatalytic process of N2RR, thus revealing the first potential-induced in situ formation of the real electrocatalytic active sites to boost the conversion of N2 to NH3. Moreover, the key intermediate of Fe-NNHx was detected experimentally by both operando XAS and in situ attenuated total reflection–surface-enhanced infrared absorption spectra (ATR-SEIRAS), indicating the alternating mechanism followed by N2RR on such catalyst. The results indicate the necessity of considering the potential-induced restructuring of the active sites on all kinds of electrocatalysts for such as highly efficient ammonia production from N2RR. It also paves a new way for a precise understanding to the structure-activity relationship of a catalyst and helps the design of highly efficient catalysts.
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ChemSusChem
·
2023
·Vol. 16
·期 17
·e202300633
·
IF 8.4
Wen Guo,Tao Yang,Hongyan Zhang,Hao Zhou,Maoshuai He,Wenxian Wei,Wenjie Liang,Yilin Zhou,Tingting Yu,Hong Zhao
Graphical A thick Ni-based catalyst layer derived from nickel foam was synthesized by a Fe 3+ -induced strategy. In addition to the remarkable conductivity, high stability and more accessible active sites, Mo,Fe co-modulation also optimizes the adsorption free energies of the OER intermediates, boosting the catalytic activities. A highly active catalyst for the oxygen evolution reaction (OER) is critical to achieve high efficiency in hydrogen generation from water splitting. Direct conversion of nickel foam (NF) into nickel-based catalysts has attracted intensive interest due to the tight interaction of the catalysts to the substrate surface. However, the catalytic performances are still far below expectation because of the problems of low catalyst amount, thin catalyst layer, and small active area caused by the limitations of the synthesis method. Herein, we develop a Fe 3+ -induced synthesis strategy to transform the NF surface into a thicker catalyst layer. In addition to the excellent conductivity and high stability, the as-prepared FeMo-Ni 2 P 2 O 7 /NF catalysts expose more active sites and facilitate mass transfer due to their thicker catalyst layer and highly dense coral-like micro-nano structure. Furthermore, the Mo, Fe co-modulation optimizes the adsorption free energies of the OER intermediates, boosting catalytic activities. Its catalytic activity is among the highest, and it exhibits a small Tafel slope of 34.71 mV dec −1 and a low overpotential of 161 mV for delivering a current density of 100 mA cm −2 compared to reported Ni-based catalysts. The present strategy can be further used in the design of other catalysts for energy storage and conversion.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yongpan Shan,Yajie Ma,Changcai Wu,Xiangliang Ren,Xianpeng Song,Dan Wang,Hongyan Hu,Xiaoyan Ma,Yan Ma
Control release of pesticides based on target plant characteristics is highly desirable for improving the effective utilization rate and reducing non-target organism risks. Here, the controlled release formulations (Cu-CS@IN@MIL-100 (Fe)) were successfully prepared by employing MIL-100 (Fe) as the carrier material, indoxacarb (IN) as the model pesticide, and chitosan (CS) as a coating to chelate copper ions by chemical crosslinking. The prepared Cu-CS@IN@MIL-100 (Fe) had an acceptable loading content (36.25 %). The introduction of CS and copper ions endowed it with sustained release properties under weak acidity conditions like cotton leaves. The laboratory bioassay experiments showed that Cu-CS@IN@MIL-100 (Fe) had practical good insecticidal activity (LC 50 = 4.936 mg/L) in controlling Helicoverpa armigera larvae. For long-term control efficacy experiments, after 14 days of application, the Cu-CS@IN@MIL-100 (Fe) treatment (73 %) mortality of Helicoverpa armigera larvae was significantly higher than the 15 % indoxacarb suspension concentrates (SC) treatment (27 %). Moreover, Cu-CS@IN@MIL-100 (Fe) had no adverse effect on cottonseed germination and the acute toxicity to Chrysopa pallens larvae was significantly lower than IN SC. Therefore, MIL-100 (Fe) could be used as an ecological safety carrier for pesticide delivery to improve IN effective utilization and reduce non-target organism risks.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jianqing Ma,Nanzhengfang Jia,Huixia Jin,Sijing Yao,Kefeng Zhang,Yin Kai,Wenliang Wu,Yuezhong Wen
The removal of Cr(VI) from wastewater still faces many challenges. This study reports on chitosan-induced synthesis of few-layer MoS 2 /Fe-doped biochar (Mo-Fe 0.5 -CS) with dual applications in Cr(VI) removal. Using chitosan as a soft template, the MoS 2 in the composite had only about 3 layers with an interlayer spacing greater than that of pure MoS 2 , while Fe was embedded in the carbon skeleton in the form of 6-coordination with O/N. The Mo-Fe 0.5 -CS composite showed high affinity for Cr(VI), with rapid adsorption reaching 100% removal within 15 min for a single solution of Cr(VI). It follows the Langmuir isotherm model with a maximum adsorption capacity of up to 180 mg/g. Furthermore, the Mo-Fe 0.5 -CS composite demonstrated catalytic activity for Fenton-like reactions, which allowed for the simultaneous removal of organic pollutants and Cr(VI). In a mixture solution of Cr(VI) and Acid Red 73 (AR73), the removal efficiencies using Mo-Fe 0.5 -CS and H 2 O 2 in 30 min were 99.7% and 96.6%, respectively. The MoS 2 acted as a cocatalyst to improve the reduction of Fe(III), and the catalysis of Cr(VI) also contributed to the removal of AR73 to a certain extent. Even at pH 10, the system was effective due to the 1 O 2 produced in the reaction and the acidic microenvironment constructed by unsaturated S atoms. These findings provide insights into the effective removal and utilization of Cr(VI) in wastewater treatment .
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yuan-li Wang,Tong-hui Yang,Song Yue,Hang-bo Zheng,Xiao-pan Liu,Peng-zhao Gao,Hang Qin,Han-ning Xiao
Composition optimization, structural design, and introduction of external magnetic fields into the catalytic process can remarkably improve the oxygen evolution reaction (OER) performance of a catalyst. NiFe2O4@(Ni, Fe)S/P materials with a heterogeneous core–shell structure were prepared by the sulfide/phosphorus method based on spinel-structured NiFe2O4 nanomicrospheres. After the sulfide/phosphorus treatment, not only the intrinsic activity of the material and the active surface area were increased but also the charge transfer resistance was reduced due to the internal electric field. The overpotential of NiFe2O4@(Ni, Fe)P at 10 mA cm–2 (iR correction), Tafel slope, and charge transfer resistance were 261 mV, 42 mV dec–1, and 3.163 Ω, respectively. With an alternating magnetic field, the overpotential of NiFe2O4@(Ni, Fe)P at 10 mA cm–2 (without iR correction) declined by 45.5% from 323 mV (0 mT) to 176 mV (4.320 mT). Such enhancement of performance is primarily accounted for the enrichment of the reactive ion OH– on the electrode surface induced by the inductive electric potential derived from the Faraday induction effect of the AMF. This condition increased the electrode potential and thus the charge transfer rate on the one hand and weakened the diffusion of the active substance from the electrolyte to the electrode surface on the other hand. The OER process was dominantly controlled by the charge transfer process under low current conditions. A fast charge transfer rate boosted the OER performance of the catalyst. At high currents, diffusion exerted a significant effect on the OER process and low OH– diffusion rates would lead to a decrease in the OER performance of the catalyst.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Huimei Shan,Huinan Mo,Yunquan Liu,Chunya Zeng,Sanxi Peng,Hongbin Zhan
Graphene oxide chitosan composite (GOCS) is recognized as an environmentally friendly composite adsorbent because of its stability and abundant functional groups to adsorb heavy metals, and Fe-Mn binary oxides (FMBO) have attracted increasing interest due to their high removal capacity of As(III). However, GOCS is often inefficient for heavy metal adsorption and FMBO suffers poor regeneration for As(III) removal. In this study, we have proposed a method of dopping FMBO into GOCS to obtain a recyclable granular adsorbent (Fe/Mn GOCS) for achieving As(III) removal from aqueous solutions. Characterization of BET, SEM-EDS, XRD , FTIR , and XPS are carried out to confirm the formation of Fe/Mn GOCS and As(III) removal mechanism. Batch experiments are conducted to investigate the effects of operational factors (pH, dosage, coexisting ions, etc.), as well as kinetic, isothermal, and thermodynamic processes. Results show that the removal efficiency ( R e ) of As(III) by Fe/Mn GOCS is about 96 %, which is much higher than those of FeGOCS (66 %), MnGOCS (42 %), and GOCS (8 %), and it increases slightly with the increasing molar ratio of Mn and Fe. This is because amorphous Fe (hydro)oxides (mainly in the form of ferrihydrite) complexation with As(III) is the major mechanism to remove As(III) from aqueous solutions, and it is accompanied by As(III) oxidation mediated by Mn oxides and the complexation of As(III) with oxygen-containing functional groups of GOCS. Charge interaction plays a weaker role in As(III) adsorption, therefore R e is persistently high over a wide range of pH values of 3–10. But the coexisting PO 4 3− can greatly decrease R e by 24.11 %. As(III) adsorption on Fe/Mn GOCS is endothermic and its kinetic process is controlled by pseudo-second-order with a determination coefficient of 0.95. Fitted by the Langmuir isotherm, the maximum adsorption capacity is 108.89 mg/g at 25 °C. After four times regeneration, there is only a slight decrease of <10 % for the R e value. Column adsorption experiments show that Fe/Mn GOCS can effectively reduce As(III) concentration from 10 mg/L to <10 μg/L. This study provides new insights into binary polymer composite modified by binary metal oxides to efficiently remove heavy metals from aquatic environments.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Dazhong Yang,Manyu Shi,Juan Zhang,Atsushi Sasaki,Masatoshi Endo
Arsenic-contaminated red mud (As-RM) is a hazardous waste with limited recycling approaches. Generally, through reductive roasting and magnetic separation, RM could be transformed into Fe-rich concentrate for Fe resource recovery. However, due to the poor thermostabilization of As species, reductive roasting of As-RM would cause severe As volatilization pollution together with high As leaching risks from heated residue. Herein, a novel johnbaumite-based As thermostabilization strategy is developed for clean Fe resources recycling from As-RM. We found that in the presence of Ca(OH) 2 , the As species in As-RM could be immobilized as thermostable and insoluble johnbaumite (Ca 5 (AsO 4 ) 3 OH) at 900 °C, effectively enhancing the As thermostability and insolubility. Introducing 1.5% Ca(OH) 2 into As-RM suppressed the As volatilization ratio from 60.3% to 15.7% during reductive roasting. Meanwhile, the As leaching concentration of the reduced residue was reduced to < 100 µg/L, thus satisfying the Japanese wastewater discharge standard. A concentrate with approximately 67.5% total iron grade was obtained from As-RM through this clean reductive roasting and magnetic separation. Overall, the approach introduced in this work effectively reduces the As diffusion pollution deriving from As-RM thermal reduction, which could contribute to hazardous As-RM reutilization, clean Fe resources recovery, and As pollution mitigation.
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