CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Wenjing Chen,Huan Tang,Han Li,Yu Zhao,Xiaozhi Wang,Jiachao Chen,Zhihui Chen,Yaxian Zhu,Wenlan Yang
Fluoride contamination is a serious problem of global concern, and water decontamination from fluoride remains an imperative but also a challenging task. Recently, Ce-Fe bimetal oxyhydroxides (CFBOs) nanoparticles of sufficient hydroxyl group and high reactivity have exhibited unique advantages for specific fluoride elimination. Unfortunately, they are difficult to apply directly in scale-up water treatment due to their ultrafine nature. Herein, we fabricated a novel polymer-based Ce-Fe bimetal oxyhydroxides nanocomposite, i.e., CFBOs@201, by co-precipitation of Ce/Fe oxides nanoparticles inside a porous polystyrene anion exchanger D201. The material characterization results confirmed that CFBOs were successfully immobilized inside the pores of D201 with nanoscale and micro crystalline nature, and the shielding effect of the host D201 significantly improved the chemical stability of CFBOs against pH variation (3–12). As compared with cerium and ferric (hydr)oxides nanocomposites (HCO@201 and HFO@201) and its host D201, CFBOs@201 exhibited superior capacity and better selectivity for fluoride adsorption. Thanks to the inner-sphere complexation between immobilized CFBOs and fluoride, the concomitant competing anions exerted negligible effect on the defluoridation efficiency of CFBOs@201. Fluoride uptake onto CFBOs@201 agreed well with the pseudo-second-order kinetic model and the Langmuir isotherm model, and the calculated maximum adsorption capacity was 65.99 mg/g. The exhausted CFBOs@201 could be efficiently regenerated by a simple alkaline treatment for cyclic utilization with constant defluorination performance. Fixed-bed assays demonstrated that the encapsulating of CFBOs nanoparticles enhanced the effective treatment capacity of CFBOs@201 by 10–12 times over the host D201 irrespective of whether synthetic wastewater or mine drainage was the feeding solution. The above results verified that CFBOs@201 is a new kind of efficient defluoridation adsorbent with practical application prospect.
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Catalysis Science & Technology
·
2022
·Vol. 13
·期 2
·468-478
·
IF 6.177
Xinyu Lu,Xiaoli Gu
The chemical demand for alkyl phenols (mainly extracted from fossil-derived resources) has been increasingly growing, which has accelerated global energy shortages. Due to the inherent aromaticity of lignin, its effective conversion into alkyl phenols is central to its adoption as a sustainable precursor to produce biochemicals. In this study, catalytic transfer hydrogenation (CTH) of alkali lignin was carried out in a mixed medium (isopropanol/formic acid) at 240 °C for 8 h over a series of bimetallic Ni based catalysts. The acidity and reducibility of the as-prepared catalysts are enhanced via WO3 introduction (to form a WO3–Al2O3 mixed support) and a bimetallic synergistic effect, respectively, leading to improved catalytic activity and selectivity towards alkyl phenols. Different kinds of phenolic compounds (e.g., those with substitutions of methoxyl, alkyl, alkenyl, carbonyl, carboxyl, or hydroxyl groups) were generated over these bimetallic Ni based catalysts with various combinations of Ni + Fe/Zn/Co/Mo/Cu, which was due to their own catalytic promotion of certain reactions (e.g., hydrogenation, deoxygenation, and/or hydrogenolysis). Reaction mechanisms of lignin depolymerization were proposed according to the distribution of phenolic compounds. This work provides a comprehensive investigation on yielding alkyl phenols from lignin CTH over a series of inexpensive bimetallic Ni based catalysts (Ni/(Fe/Zn/Co/Mo/Cu)–WO3/Al2O3), and undertook a catalytic evaluation of the bimetallic synergistic effects on improving the chemical selectivity towards alky phenols, which is beneficial for lignin valorization.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiahang Qiu,Zhen Xin,Mu Zhang,Xudong Sun
Due to the multiple scattering of microwaves and the existence of electron aggregation polarization at heterogeneous interfaces, the design of hollow or anisotropic microstructures has always been one of the research focuses of microwave absorption materials (MAMs). In this work, an effective strategy has been proposed reasonably to manufacture yolk-shell pompon-like Fe@void@CeO 2 @Ni nanospheres via hydrogen reduction and multiple solvothermal procedures. The results show that the metallic iron core with a diameter of 300 nm and the outer CeO 2 layer with a thickness of 70 nm compound to form a yolk-shell structure, and the metallic nickel nanosheets with a length of about 100 nm are evenly embedded in the CeO 2 layer to form a pompon-like structure. These unique microstructures provide heterogeneous interfacial polarization, three-dimensional conductive networks, and multiple electromagnetic scattering which bring excellent dielectric loss to the composites. Combined with the inherent strong magnetic loss of magnetic metals, as-prepared composites exhibit excellent microwave absorption properties. The minimal RL value reaches −48.9 dB and the efficient absorption bandwidth reaches 14 GHz with the thickness ranges from 2.5 to 7 mm. Hence, this unique microstructural design scheme has great prospects in the field of MAMs.
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ELECTROANALYSIS
·
2023
·Vol. 35
·期 5
·e202200521
·
IF 3
Luyi Chen,Ping Xiao,Bin Hu,Yiwen Wang,Jianmao Yang,Jianyun Liu
3-dimensional (3D) Fe−Co−LDH/MXene composite was synthesized by in-situ synthesis and assembly of Fe−Co−LDH rod around MXene under hydrothermal condition. Due to the unique 3D configuration and good conductivity, the obtained Fe−Co−LDH/MXene modified glassy carbon electrode (Fe−Co−LDH/MXene/GCE) showed excellent electrochemical activity for As(III) detection. Via square-wave anodic stripping voltammetry, the response current on Fe−Co−LDH/MXene/GCE had good linear relationship with As(III) concentrations (1∼1000 ppt) with superior sensitivity (0.22 μA ppt −1 cm −2 ) and low detection limit (0.9 ppt). The mechanism of As(III) adsorption was demonstrated. The electrode showed excellent anti-interference ability. Real water sample analysis demonstrated the Fe−Co−LDH/MXene/GCE was deployable in aqua-system.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yang Wang,Shiyuan Lin,Meng Li,Chuanyong Zhu,Hao Yang,Pei Dong,Mingjie Lu,Wenhang Wang,Jianlin Cao,Qiang Liu,Xiang Feng,Han Hu,Noritatsu Tsubaki,Mingbo Wu
The direct transformation of CO 2 into valuable chemicals with the aid of sustainable energy-generated H 2 has attracted enormous interest owing to the integrated functions of carbon elimination and non-fossil fuel-derived products supply. As one of the most promising catalysts for CO 2 hydrogenation, the chemical properties of Fe-based catalysts, such as electronic structure and coordination environment, have been widely studied. However, the mass/heat transfer effects in Fe-based catalysts are also crucial to the targeted product selectivity and catalytic stability, but have been rarely investigated due to the lack of facile fabrication protocols. Herein, we precisely fabricate and tailor the architecture of the Fe-based monolithic catalysts by a direct ink writing (DIW)-type three-dimensional (3D) printing technology under the guidance of the computationally controlled printing procedure. The Fe-based monolithic catalyst with spiral-type architecture delivers extremely high light olefins selectivity (52.6%) and space time yield (STY, 451.8 g CH2 kg cat −1 h −1 ) from CO 2 hydrogenation. Based on the mass-transfer simulation, the spiral-structured channels in the Fe-based monolithic catalyst lower the coverage of intermediates and products on the catalytic interface due to the optimal mass-transfer effect, thus maximizing the utilization of active sites and timely terminating the carbon-chain growth. More in-depth, the density functional theoretical (DFT) simulations verify that the relatively electron-rich catalytic interface with low intermediate coverage could facilitate the desorption of olefins and decelerate the C-C coupling step, which synergistically guarantee the enhanced light olefins synthesis performance. Furthermore, the enhanced heat-transfer effect endowed by the 3D architecture prolongs the life-time of catalyst by avoiding undesirable active site aggregation and carbon deposition. The powerful strategy for catalyst fabrication not only provides a new concept of regulating the CO 2 hydrogenation performance of Fe-based catalysts but also holds a great promise to spread into other catalytic systems for targeted synthesis.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Tianliang Xia,Meiting Ju,Hengli Qian,Xinyu Bai,Ruite Lai,Chao Xie,Guanjie Yu,Yao Tang,Chengxu Wang,Qidong Hou
Peroxymonosulfate (PMS) activation is a prospective technique for pollutant degradation, but less attention has been paid to the tunable modulation and effective utilization of reactive oxygen species in selective oxidation. Herein, we develop a photocatalytic Fenton-like system with Fe single-atom supported on carbon nitride that generates singlet oxygen ( 1 O 2 ) as dominant active species to selectively oxidize glucose to gluconic acid. The loading of atomic Fe onto carbon nitride can notably aggrandize the light absorption and boost the photon-generated carriers transfer efficiency. With PMS and simulated sunlight, the Fe single-atom catalyst afforded a glucose conversion of 36.3% with gluconic acid selectivity up to 91.6%, as is superior to the state-of-the-art catalytic systems. Control experiments and theoretical analysis reveal that the excellent catalytic performance of Fe single-atom supported on carbon nitride is resulted from the enhanced photocatalytic activity with better PMS activation ability.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2023
·
IF 4.1
Meiling Zhan,Minghao Fang,Liangyu Li,Yajing Zhao,Bozhi Yang,Xin Min,Pengpeng Du,Yan'gai Liu,Xiaowen Wu,Zhaohui Huang
In the pursuit of enhancing the property of photocatalytic hydrogen production , strategies for enhancing light absorption and the separation and transport efficiency of photo-induced carriers have been studied. Perovskite photocatalyst has great application potential in the field of photocatalytic hydrogen production due to its special crystal structure. LaMn (1-x) Fe x O 3 (x = 0–0.08) perovskite nanofibers with diameters of 50–200 nm were synthesized by electrospinning, and their photochemical properties were investigated. The results of UV–Vis diffuse reflectance spectroscopy, PL spectroscopy, I-t, and EIS revealed that the doping with Fe could improve light absorption and reduce the recombination rate of photogenerated electron-hole pairs, and improve the separation and transfer efficiency of photogenerated electron-hole pairs, likely due to the increased concentration of oxygen vacancies caused by doping. Through optimization of the Fe doping amount, an improved hydrogen production efficiency of 767.71 μmol h −1 g −1 was achieved for LaMn 0·96 Fe 0·04 O 3 , which is 2.5 times the efficiency of undoped LaMnO 3 (300.74 μmol h −1 g −1 ). These results provide a new idea for the development of efficient photocatalysts for hydrogen production.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Haiyan Wang,Yanan Chen,Wenfu Xie,Xiaoxue Han,Qian Feng,Rong Jiang,Hu Shang,Feifei Zhang,Linna Gao,Zonghua Wang
A novel Pt/Ni-Fe layered double hydroxide (Pt/Ni-Fe LDH) electrocatalyst was fabricated by a two-step facile process for oxidation of methanol in alkaline medium. It is found that Pt/Ni-Fe LDH electrocatalyst exhibits higher electrocatalytic activity, better anti-poisoning ability and stability for methanol oxidation comparing to pure Pt black and commercial Pt/C catalyst. Such an enhancement is probably attributed to the synergistic effect of Ni-Fe LDH and the uniform loading of Pt nanoparticles on the LDH layers. When ionic liquid (IL) was introduced to the composites, the prepared Pt/IL/Ni-Fe LDH exhibits even better electrocatalytic behaviors (205.6 mA mg -1 Pt, I f /I b=5.67) than the Pt/Ni-Fe LDH. Moreover, the morphology and structure of composites were characterized using scanning electron microscope equipped with an energy dispersive X-ray spectrometry, transmission electron microscope, X-ray diffraction, and FT-IR spectra. It is found that the Ni-Fe LDH have a flake-like morphology, the mean diameter of Pt nanoparticles in Pt/Ni-Fe LDH and Pt/IL/Ni-Fe LDH electrocatalyst is 4.36 nm and 3.09 nm, smaller than that in pure Pt black and commercial Pt/C electrocatalyst (8.70 nm and 6.48 nm).
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·
IF 5.8
Zhong Dengjie,Liu Peng,Liu Yi,Xu Yunlan
The Zn/Fe@N-doped porous graphitic carbon catalyst (Zn/Fe@PCN) was successfully produced through one-step pyrolysis of g-C 3 N 4 and Zn/Fe-MOF and was used for the activation of persulfate (PS) for the degradation of RhB. The Zn/Fe@PCN/PS system was able to degrade 95.92% of RhB in 30 min at a rate of 0.6453 min −1 when RhB was concentrated at 50 mg L −1 . The efficient degradation of RhB is primarily realized through the synergistic activation of PS by Zn, Fe, and N to produce reactive oxygen species 1 O 2 , \(\cdot{\mathrm{O}}_2^-\) , \(\cdot \mathrm{SO}_4^-\) , and ·OH. Zn 0 /Fe 0 in Zn/Fe@PCN forms a galvanic cell with carbon to release electrons to join in the activation of PS. The doping of Zn not only provides sufficient electrons for the activation of PS but also promotes the effective reduction of Fe 2+ and thus the Fe 2+ /Fe 3+ cycle. The N doping accelerates the electron transfer during the reaction progress.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fengliang Cao,Qingshan Zhao,Debin Kong,Xiaojie Tan,Xinxin Li,Tengfei Liu,Linjie Zhi,Mingbo Wu
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts show great potential for heterogeneous catalysis. However, recognizing and engineering the microenvironment of M-N x sites to achieve satisfactory catalytic performance remains challenging. Herein, we propose a facile g-C 3 N 4 -assisted template strategy to anchor atomic Fe-N 4 sites on highly nitrogen-doped carbon nanosheets. Through regulating the ratio and type of peripheral nitrogen species by carbonization temperature, the optimal Fe-N-C-800 catalyst showed significantly boosted catalytic activities (overall turnover frequency of 13.43 min −1 and activation energy of 19.44 kJ mol −1 ) for nitroarene reduction with extremely low reductant dosage, exceeding most reported metal catalysts. Experimental and theoretical results reveal appropriate graphitic- and pyrrolic-N dopants surrounding the Fe-N 4 center can tailor the local electronic structure and contribute to obvious upshift of the d-band center, which dramatically promotes the adsorption and conversion of reactant substrates, eventually delivering the unprecedented catalytic performance. This work provides a guide for rational coordination environment regulation of single-atom catalysts for efficient chemical transformations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Linfang Cui,Jie Hao,Yan Zhang,Xiaomin Kang,Jiujun Zhang,Xian-Zhu Fu,Jing-Li Luo
Fe-, and N-co-doped carbon (Fe N C) electrocatalysts are promising alternatives to Pt-based catalysts for oxygen reduction reaction (ORR); however, simultaneously enhancing their intrinsic activity and exposure of Fe active sites remains challenging. Herein, we report S-modified Fe single-atom catalysts (SACs) anchored on N,S-co-doped hollow porous nanocarbon (Fe/NS-C) for ORR. The unique hollow structure and large surface area of the SACs are favorable for mass/electron transport and exposure of Fe single-atom active sites. The as-prepared Fe/NS-C electrocatalysts display a high-efficiency ORR activity with a half-wave potential of 0.893 V versus the reversible hydrogen electrode and exceed that of the benchmark commercial Pt/C catalyst as well as most reported transition-metal based SACs. Impressively, the Fe/NS-C-based Al-air battery (AAB) displays a high open circuit voltage of 1.48 V, a maximum power density of 140.16 mW cm −2 , and satisfactory durability, outperforming commercial Pt/C-based AAB. Furthermore, Fe/NS-C exhibits considerable potential as a cathode catalyst for application in direct methanol fuel cells. Experimental and theoretical calculation results reveal that the excellent ORR performance of Fe/NS-C can be contributed to the highly active FeN 3 S sites and the unique hollow structure. This work provides new insights into the rational design and synthesis high-performance ORR electrocatalysts for energy conversion and storage devices. of employing ZIF-8 as precursors.
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高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Heng Shi,Yi He,Yubin Li,Pingya Luo
Fenton-like catalysis based on peroxymonosulfate (PMS) activation has shown great potential in the treatment of organic wastewater. Heterogeneous Fenton-like catalysts containing transition metal active sites are highly efficient for PMS activation. However, the reduction of oxidized metal active sites was usually not prompt due to the sluggish reaction kinetics, which caused the insufficient redox cycle of the metal active sites and further hampered the catalysis efficiency. Recent studies have shown that the synergy effect between photocatalysis and PMS activation may address the above obstacle and boost overall efficiency. However, a deeper understanding of this synergy effect is still missing, making it difficult to be rationally controlled; thus, a poor synergy effect is frequently reported. Herein, a Co/Fe bimetal-doped graphitic carbon nitride (g-C3N4) was designed representatively through systematical characterization and theoretical calculation, the synergy effect was revealed to be profoundly determined by the competitive role of a hole in the system and the adsorbed metastable PMS* on the catalyst surface, and furthermore, the synergy effect can be rationally manipulated; when the Co/Fe doping ratio is 2.5:2.5, the as-prepared g-C3N4 with a moderate valence band position can endow the catalyst with an optimized photo-Fenton-like synergistic effect and the highest catalytic degradation performance. This work sheds light on the rational design of highly efficient photo-Fenton-like catalysts.
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