CHEMISTRY-A EUROPEAN JOURNAL
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2021
·Vol. 27
·期 35
·9031-9037
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IF 5.236
Yibo Zhang,Yuying Zheng,Hongbo Geng,Yang Yang,Minghui Ye,Yufei Zhang,Cheng Chao Li
Graphical Novel structured M 2 P 2 O 7 /C (M=Fe, Co, Ni) nanoflake composites are prepared via an organic-phosphors precursor assisted solvothermal method and a post high temperature annealing process, which could deliver superior potassium storage performance. Metal phosphates have been widely explored in lithium ion batteries and sodium ion batteries owing to high theoretical capacities, mild toxicity and low cost. However, their potassium ion battery applications are less reported due to the limited conductivity and the slow diffusion kinetics. Considering these drawbacks, novel structured M 2 P 2 O 7 /C (M=Fe, Co, Ni) nanoflake composites are prepared through an organic-phosphors precursor-assisted solvothermal method and a subsequent high temperature annealing process. The designed Co 2 P 2 O 7 /C composite exhibits the highest rate capacity with 502 mAh g −1 at 0.1 A g −1 and good cyclability for 900 cycles at 1 A g −1 and 2 A g −1 when compared with Ni and Fe based composites. The superior electrochemical performance can be attributed to their unique nanoparticle-assembled nanoflake structure, which can afford enough active sites for K + intercalation. In addition, the robust pyrophosphate crystal structure and the in situ formed carbon composition also have positive effects on enhancing the long-term cycling performance and the electrode's conductivity. Finally, this organic-phosphors precursor induced simple approach can be applied for easy fabrication of other pyrophosphate/carbon hybrids as advanced electrodes.
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CHINESE JOURNAL OF CATALYSIS
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2021
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IF 8.271
Jun-Sheng Jiang,He-Lei Wei,Ai-Dong Tan,Rui Si,Wei-De Zhang,Yu-Xiang Yu
Iron-based single-atom catalysts with nitrogen-doped carbon as support (Fe-SA/NPC) are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells. However, synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging. Herein, we report a high-loading (7.5 wt%) Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes. Both the nitrogen-doped porous carbon (NPC) support with high specific surface area and ο -phenylenediamine ( o -PD) play key roles role in the preparation of high-loading Fe-SA/NPC catalysts. The results of X-ray photoelectron spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates (Fe-N 4 ). The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading. The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V. Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Jiang-Bo Huo,Guoce Yu
Efficient elimination of As(III) from drinking water and wastewater has been a challenge because of its neutral molecular form. To address this problem, a novel nanocomposite , mesoporous cerium oxide-anchored magnetic polyhedrons derived from MIL-100(Fe) was fabricated via a strategy combining impregnation and calcination . The resultant products (denoted as Fe 2 O 3 /CeO 2 -t) exhibited a unique octahedral nanostructure decorated by mesoporous cerium oxide . Surface modification of CeO 2 enhanced As(III) removal in comparison to unmodified Fe 2 O 3 . Particularly, Fe 2 O 3 /CeO 2 -4 h can reduce As(III) concentration from 180 to 10 µg/L within 20 min, which was almost 9 times faster than unmodified Fe 2 O 3 . The adsorption behavior conformed to the pseudo-second-order kinetic model ( R 2 = 0.9908) and the Freundlich isotherm model ( R 2 = 0.9943). The maximum adsorption capacity of As(III) by Fe 2 O 3 /CeO 2 -4 h was 68.25 mg/g, higher than those reported for similar adsorbents. Its enhanced removal mechanism can be attributed mainly to the mesoporous characteristics and oxidization ability of surface ceria. The composite can be separated from water by external magnets and easily regenerated. This study may offer a clue to the design of metal-organic framework-based composites as an alternative adsorbent for arsenite cleanup.
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Nanoscale
·
2021
·Vol. 13
·期 31
·13463-13472
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IF 7.79
Ya-Nan Zhou,Ruo-Yao Fan,Yu-Ning Cao,Hui-Ying Wang,Bin Dong,Hui-Ying Zhao,Fu-Li Wang,Jian-Feng Yu,Yong-Ming Chai
The oriented distribution and strong bonding of Fe active sites in multiple metal hydroxides are crucial to modulate activity and stability for efficient oxygen evolution reaction (OER). However, the dispersion and inevitable dissolution of Fe species still need to be addressed through deliberate design. Here, trace amounts of Fe chelated with tannic acid (TA) are precisely anchored to ultrathin Co hydroxides (TF@Co(OH)2-t) through a new anodic interfacial coordination assembly strategy: firstly, the ZIF-67@Co(OH)2 precursor with ultrathin Co(OH)2 nanosheets vertically grown on the shell, provides abundant active sites and sufficient anchoring regions for subsequent TA–Fe coating; secondly, the TA–Fe ligand network quickly and robustly coats the surface of the Co(OH)2via positive potential-driven chronopotentiometry, yielding TF@Co(OH)2-t with good dispersion and controllable Fe species. The TA–Fe network efficiently activates Co species and prevents the dissolution of Fe ions. Physical characterization and DFT simulations reveal that the optimized OER activity with 317 mV at 10 mA cm−2 for TF@Co(OH)2-500 can be attributed to the accelerated electron transfer, increased active sites, and the moderate fall in d-band center levels due to Fe integration. Moreover, prolonged stability is realized benefiting from the robust TA–Fe coating protecting the actives sites.
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FUEL
·
2021
·
IF 6.609
Jiaxing Wang,Shuping Zhang,Yinhai Su,Shuguang Zhu
Carbon-based metal catalyst has attracted wide attention in the utilization for tar catalytic cracking because of its high hierarchical porous structure and high dispersion of metal particles. In this study, sawdust was used as raw material to prepare Fe embedded graphene nanoshell/carbon nanofibers catalyst for catalytic cracking of biomass tar by impregnation followed by carbothermal reduction in CO 2 atmosphere. The properties of the catalysts were evaluated by a variety of characterization methods and based on which the evolutionary mechanism was proposed. CO 2 etching improved the porosity (V total = 0.4187 cm 3 /g and BET surface area = 225.93 m 2 /g) and increased the content of Fe 0 . During CO 2 etching and catalysis of FeCl 3 , the prepared catalyst formed a structure in which a large amount of carbon nanofibers/graphene shells wrapped metallic iron deposited on the porous carbon support. The stacking of carbon nanofibers enhanced the adsorption capacity of the catalyst to tar macromolecules. The coating of the graphene shell to the metal nanoparticles prevented the agglomeration and sintering of metal active sites, which increased the stability of the catalyst. The results indicated that the Fe@C800C1 catalyst showed good catalytic performance at 700 °C, and the tar conversion efficiency reached up to 90.4%. After 4 cycles, the tar removal efficiency still maintained at 90.0%.
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ENERGY
·
2021
·
IF 7.147
Xiuquan Li,Zhongqing Yang,Li Zhang,Ziqiang He,Ruiming Fang,Ziqi Wang,Yunfei Yan,Jingyu Ran
The catalytic reaction of C 2 H 6 with CO 2 provides an opportunity to use shale gas and the greenhouse gas as source materials to produce ethylene through oxidative dehydrogenation or produce syngas through dry reforming . In this work, the reaction characteristics of ethane with CO 2 on Fe/Co/Ni/Cu monometallic catalysts and Pd-doped bimetallic catalysts were studied through activity test, kinetic analysis , catalyst characterization and DFT calculation. It is found that Pd–Fe 6 /CeO 2 has a high and stable C 2 H 4 selectivity of 80.4%, which is suitable for oxidative dehydrogenation reaction, while Ni 6 /CeO 2 has a large ethane/CO 2 conversion and a high CO selectivity of 96.5%, which is suitable for dry reforming reaction. For Fe-based catalyst, the doping of Pd form double active component structure. It only reduces the energy barrier of ethylene formation and CO 2 direct activation to provide O∗, but also increases the energy barrier of ethylene deep dehydrogenation, thus increasing the conversion of reactants and selectivity of C 2 H 4 . For Ni-based catalysts, the doping of Pd forms the alloy structure, which reduces the energy barrier of O∗-assisted dehydrogenation reaction and increases the conversion of reactants, but increases the energy barrier of C–C bond cleavage and CO 2 activation reaction, which reduces the selectivity of reforming to syngas.
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SOLID STATE SCIENCES
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2021
·
IF 3.059
Cong Huang,Jun Wang,Mengjun Li,Xiaofang Lei,Qiang Wu
The construction of Z-scheme systems is a valid strategy to effectively enhance photocatalytic property in the field of photocatalysis . In the present work, a novel Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was prepared via a simple one-pot solvothermal method for the first time. The phase structure, morphology and optical property of the as-prepared V 2 O 5 /NH 2 -MIL-101(Fe) composite were carried out by a series of characterizations. The photocatalytic property of V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was investigated by photodegrading tetracycline (TC) under ultraviolet–visible light irradiation. The systematic studies indicate that the obtained V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst possesses superior photocatalytic performance toward TC removal. Furthermore, a Z-scheme photocatalytic degradation mechanism for TC over V 2 O 5 /NH 2 -MIL-101(Fe) composites was proposed. The results show that Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst has potential application in the treatment of TC wastewater. This research will broaden the studies of NH 2 -MIL-101(Fe)-based Z-scheme photocatalysts.
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NANO
·
2021
·
IF 1.556
Jungang Yi,Kun Wu,Huadong Wu,Jia Guo,Linfeng Zhang,Hao Li,Jianding Li
The presence of the antibiotics in the wastewater has posed a huge risk to aquatic life and human health. It is a great significance to develop an effective technology to treat the antibiotics-containing wastewater. In this study, a series of g-C 3 N 4 /NH 2 -MIL-88B(Fe) composite photocatalysts are synthesized through a simple one-step method. The structure and optical properties of prepared photocatalysts are detected by X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–Vis absorption spectra (UV–Vis DRS), photoluminescence (PL) spectroscopy and transient photocurrent techniques, respectively. FESEM and TEM show that MOF is uniformly dispersed in petaloid g-C 3 N 4 . The uniform dispersion of Fe-MOFs in the heterojunction composites increases the specific surface area ( S BET ) of g-C 3 N 4 , which results in a great adsorption property for the nanocomposite. The capture experiment shows that • O 2 − and h + are the main active substances in ciprofloxacin (CIP) degradation. These prepared composite photocatalysts exhibit excellent CIP photodegradation activity under visibly light irradiation with an apparent rate constant of 0.0127 min − 1 (3.74 times as the rate of single component). The remarkable catalytic performance can be ascribed to the fact that the g-C 3 N 4 /NH 2 -MIL-88B(Fe) heterojunction inhibits the recombination of photoinduced electron–hole pairs and improved the visible light absorption.
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Catalysts
·
2020
·Vol. 10
·期 11
·1329
·
IF 3.52
Shijie Hao,Yandi Cai,Chuanzhi Sun,Jingfang Sun,Changjin Tang,Lin Dong
Monolithic Mn-Fe-Ce-Al-O catalyst with honeycomb cordierite ceramic as a carrier was reported for the first time for low temperature deNOxapplication. In the reaction of selective catalytic reduction (SCR) of NO with NH3, a NO conversion of above 80% at 100 °C was obtained. Notably, the catalyst also showed excellent resistance against SO2and H2O. About 60% NO conversion was maintained after successive operation in the mixed stream of SO2and H2O for 168 h. The Brunner−Emmet−Teller (BET) measurement, SEM, EDS, thermogravimetric analysis (TG), FT-IR, and XPS results of the used catalysts indicated that certain amounts of ammonium sulfate was formed on the surface of the catalyst. XPS results revealed that partial of Fe2+was oxidized to Fe3+during the reaction process, and Fe2+species have strong redox ability, which can explain the decrease in activity after reaction. In addition, SO2and H2O induced a transformation of Ce from Ce4+to Ce3+on the surface of the catalyst, which increased the amount of chemisorbed oxygen. Owing to these factors, the addition of Ce and Fe species contributes to excellent resistance of the catalyst to SO2and H2O.Keywords:honeycomb catalyst;Mn-Fe-Ce-Al-O;low temperature denitration;water and sulfur resistance
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yafu Tang,Yuechao Yang,Shanmin Hou,Dongdong Cheng,Yuanyuan Yao,Shugang Zhang,Jiazhuo Xie,Xiaoqi Wang,Xiaoxiao Ma,Zhen Yu,Shan Li
Iron (Fe) chelated by water-soluble humic substances can effectively overcome plant micronutrient deficiencies. However, the traditional synthesis methods are often complex, expensive, and thus not applicable to large-scale industrial productions. In this work, an ecofriendly and multifunctional Fe–humic acid (HA) complex was successfully prepared through simply ball milling lignite with double-shelled Fe–N hollow mesoporous carbon microspheres (DS–Fe–N–HC). The novel DS–Fe–N–HC was synthesized using a simple strategy and was first applied in activating HA from lignite by solid-phase ball milling to attain the water-soluble HA–iron fertilizer (WHIF). The physicochemical properties of the DS–Fe–N–HC nanocomposites and WHIF were systematically characterized by a series of techniques. A traditional Fe–HA complex is mainly obtained by mixing HA and iron ions, which has poor water solubility because HA is not activated. In comparison to samples prepared with other methods, WHIF contained more stable water-soluble HA. Furthermore, the as-obtained WHIF had higher amounts of proteins and amino sugar tannin as evidenced in FT-ICR MS analysis. Moreover, WHIF contributed to higher activities in chlorophyll content, height, steam diameter, and biomass of peanuts than other samples. The results demonstrate that WHIF is effective in reducing symptoms of iron deficiency in peanuts, which can be attributed to its iron-based compounds and water-soluble HA. The findings of this study provide a promising, cost-effective, and environmentally friendly solution to mitigate iron deficiency and promote the growth of peanuts for large-scale agriculture production.
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ChemSusChem
·
2021
·Vol. 14
·期 7
·1710-1719
·
IF 8.928
Liwei Shi,Hailiang Fang,Xiaoxia Yang,Jie Xue,Caifeng Li,Shifeng Hou,Cheng Hu
Graphical Doping for batteries : Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates provide elevated performance as Li−S free-standing cathodes. Fe-doping in NiSe 2 enables improved charge transfer and stronger interactions with the adsorbed sulfur species, as well as higher electrical conductivity. The transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles eliminates the barriers of phase transitions during the cathode redox processes. The commercialization of Li−S batteries is hindered by the shuttling of lithium polysulfides (LiPSs), the sluggish sulfur redox kinetics as well as the low sulfur utilization during charge/discharge processes. Herein, a free-standing cathode material was developed, based on Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates (Fe-NiSe 2 /ACC) for high-performance Li−S batteries. Fe-doping in NiSe 2 plays a key role in the electronic structure modulation of NiSe 2 , enabling improved charge transfer with the adsorbed LiPSs molecules, stronger interactions with the active sulfur species and higher electrical conductivity. Effective promotion of the sulfur redox kinetics and enhanced sulfur utilization were achieved under high areal sulfur loadings. The stronger interactions with LiPSs together with the unique 3D structure of Fe-NiSe 2 /ACC also induced the transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles, significantly eliminating the barriers of solid nucleation and growth during the phase transition of liquid LiPSs to solid Li 2 S 2 /Li 2 S. With a high sulfur loading of 9.9 mg cm −2 , the Fe-NiSe 2 /ACC cathode enabled a high area capacity of 9.14 mAh cm −2 with a low average decay of 0.11 % per cycle over 200 cycles at 0.1 C.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Tong Li,Yuheng Bao,Huiqiang Qiu,Weijun Tong
Single atom nanomaterials possess catalytic activity like natural enzymes are termed as SAzymes which have gained great attention during last two years because of the maximal utilization of atoms and the benefit of understanding structure-property relationship. However, most of SAzymes are fabricated based on hydrophobic carbon, which disperse poorly in water and exhibit inferior affinity towards substrates, which may limit their biomedical applications. Here, we report a peroxidase-like SAzyme through the post-modification route based on hydrophilic defective metal-organic frameworks. Hydrochloric acid (HCl) is employed as ligand modulator to fabricate defective NH 2 -UiO-66 nanoparticles (HCl–NH 2 -UiO-66 NPs). Compared with the NPs fabricated through acetic acid modulation method (Ac-NH 2 -UiO-66 NPs), HCl–NH 2 -UiO-66 NPs have more missing linkers. Hence, more Fe(Ⅲ) ions can be successfully doped onto Zr 6 clusters in HCl–NH 2 -UiO-66 NPs in a single atom state via formation of Fe–O–Zr bridge. The HCl–NH 2 -UiO-66 NPs doped with Fe(Ⅲ) ions (Fe–HCl–NH 2 -UiO-66 NPs) possess higher peroxidase-like activity than Fe-Ac-NH 2 -UiO-66 NPs due to the higher loading amount of Fe. Besides, both Fe–HCl–NH 2 -UiO-66 NPs and Fe-Ac-NH 2 -UiO-66 NPs exhibit lower Michaelis-Menten constants (K m ) for hydrogen peroxide (H 2 O 2 ) than most reported nanomaterials, indicating their higher affinity to H 2 O 2 . Due to their excellent catalytic activity to low concentration of substrates, Fe–HCl–NH 2 -UiO-66 NPs can detect H 2 O 2 with a limit of detection (LOD) of 1.0 μM. Thus, our system can be used to detect the low cellular H 2 O 2 concentration. With high peroxidase-like activity induced by plenty of single atom Fe(Ⅲ) sites, Fe–HCl–NH 2 -UiO-66 NPs can also find wide applications in other fields including nanomedicine , pollution degradation and catalysis.
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