Chemistry-An Asian Journal
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2023
·Vol. 18
·期 11
·e202300202
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IF 4.1
Zhenyu Zhou,Dexuan Li,Weiming Huang,Rongyue Wang,Jiapeng Zhong,Yangyang Zhang,Jiazhou Meng,Chuanhao Li
Graphical The pH value not only influences the surface charges of an adsorbent, but also affects the form of phosphate, which might decrease the adsorption efficiency of an adsorbent. Herein, an effective adsorbent was developed to realize phosphate adsorption by different adsorption mechanisms (electrostatic attraction or ligand exchange) in a wide pH range. Eutrophication has posed a threat to aquatic ecosystems, so it's urgent to remove excessive phosphate from water. In this study, we developed an adsorbent material, cerium/terephthalic-acid metal-organic-frameworks (Ce-MOF), to remove phosphate from different water systems. The optimal Ce-MOF presented a maximum phosphate adsorption capacity of 377.2 mg/g, approximately 3.7 times higher than that of the commercial phosphate adsorbent (Phoslock: 101.6 mg/g). Experimental and computational analysis suggested that pH dominated the adsorption process. The main forces driving the adsorption process changed from the synergistic effect of electrostatic attraction and ligand exchange at lower pH to only ligand exchange at the increased pH values. Hence, the Ce-MOF is applicable for phosphate adsorption in a wide pH range. Impressively, the adsorbent remained an excellent phosphate adsorption performance in the real water containing various interfering ions and organic matters, indicating the potential of Ce-MOF for the practical use to solve the water eutrophication issue.
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MATERIALS RESEARCH BULLETIN
·
2021
·
IF 4.641
Yanhua Yao,Changhai Liu,Linlin Luo,Dingwei Ji,Wenchang Wang,Zhidong Chen
To enhance the intrinsic activity and the density of active sites of the electrocatalyst for the hydrogen evolution reaction (HER), the microwave-assisted synthesis is adopted to prepare hierarchical Ce-doped MoSe 2 @CNTs as highly-efficient catalysts for HER in both acidic and alkaline conditions. The well-defined hierarchical nanostructure of Ce-doped MoSe 2 on multiple carbon nanotubes (MWCNTs) with few layers of MoSe 2 nanostructure. The Ce-MoSe 2 @CNTs sample with an optimal proportion of Ce:Mo (1:5) exhibits outstanding activity and long-term stability in both acidic and alkaline electrolyte. It shows an overpotential of 108 and 166 mV at 10 mA cm −2 in acidic and alkaline electrolyte, respectively. This study offers a prospective opportunity to design and fabricate the highly-effective catalysts coupling with multiple synergistic effect for efficient electrocatalysts.
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FUEL
·
2020
·
IF 5.578
Tongxin Qu,Shengli Niu,Xiangyu Zhang,Kuihua Han,Chunmei Lu
The calcium modified Zn-Ce/Al 2 O 3 heterogeneous base catalysts are synthesized by the hydrothermal method, impregnation method and co-precipitation method, respectively. Further, they are applied to catalyze transesterification of palm oil with methanol for the biodiesel production. The hydrothermal method with the Ca: Zn: Ce: Al molar ratio of 5: 4: 1: 1 is preferred to synthesize the catalyst due to the best catalytic performance. The catalyst shows strong reusability, where the biodiesel yield of 87.37% is obtained for the fifth reused cycle and the weakened catalytic capability is mainly ascribed to the leaching out of the active sites. The response surface methodology with the central composite design (RSM-CCD) is employed to optimize the transesterification parameters and predict the biodiesel yield. The predicted maximum biodiesel yield of 99.44% is achieved at the reaction temperature of 66.12 °C, methanol to oil molar ratio of 18.53 and catalyst amount of 8.19 wt. % with 3 h, which is consistent with the experimental result of 99.41%. Also, the physical properties of the produced biodiesel meet the ASTM D 6751 standard. This study reveals the Ca-Ce-Zn/Al 2 O 3 catalyst gains a good application prospect in the biodiesel production and the response surface methodology is effective in optimizing the transesterification parameters and predicting the optimal values.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Chao Shan,Hui Liu,Ming Hua,Bingcai Pan
The development of catalysts for oxidation of aqueous contaminants has long been relying on trial-and-error strategies due to lack of activity-tuning principles. Herein, Fenton-like oxidation of As(III) as a chemisorbed model contaminant over a series of fabricated CexTi1-xO2 catalysts with tunable structures was investigated. The activity of CexTi1–xO2 showed a volcano-shape dependency on Ce molar fraction, peaking at Ce0.25Ti0.75O2 (x = 0.25) with 6.32–6.36 times higher activity and 2.67–2.94 times higher specific activity compared with CeO2 and TiO2. The non-radical surface hydroperoxo complexes were experimentally substantiated as the dominant oxidant species on Ce0.25Ti0.75O2, which enabled a high efficiency of H2O2 utilization (99.1%). Under the verified Langmuir–Hinshelwood mechanism, the microkinetic model for the catalytic oxidation was established, and thus, the quantitative relationship between activity and adsorption energies for bimolecular chemisorption reactions was elucidated. Theoretically, a catalyst with identical adsorption energies toward both chemisorbed reactants tends to obtain the highest activity. Through DFT calculation, the highest activity of Ce0.25Ti0.75O2 was rationally interpreted by the balanced adsorption energies toward As(III) and H2O2, which was attributed to the shifted electronic density of states induced by Ce doping. This study provides a potent strategy to tune the catalytic activity of bimolecular chemisorption reactions.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaofeng Wang,Zhe Zhao,Yang Xu,Qingbo Li
A series of 3DOM-Mn x Ce y Ti z catalysts with three-dimensionally ordered macroporous (3DOM) structure were synthesized by a soft template method. The high SCR activity of the 3DOM-Mn 3 Ce 1 catalyst at low temperature was owing to the excellent redox ability and rich Lewis and Brønsted acid sites of the catalysts, which were beneficial to improve the catalytic activity. However, the strong oxidizability of MnO x resulted in the nonselective oxidation of NH 3 and generation of N 2 O, decreasing the N 2 selectivity. After addition of Ti, the redox capacity of the 3DOM-Mn 3 Ce 1 Ti 1 catalyst decreased, and the NH 3 were strongly adsorbed on the acid sites, which enhanced the N 2 selectivity with a broadened temperature window of 240–440 °C and a high GHSV of 120000 h −1 . Furthermore, both the 3DOM-Mn 3 Ce 1 and 3DOM-Mn 3 Ce 1 Ti 1 catalysts showed remarkable tolerance of H 2 O. Finally, through in situ DRIFT analysis, the Langmuir-Hinshelwood (L-H) mechanism was confirmed as the dominant reaction pathway over the 3DOM-Mn 3 Ce 1 Ti 1 catalyst.
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CHEMOSPHERE
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2018
·
IF 4.427
Zhipan Wen,Yalei Zhang,Gang Cheng,Yingru Wang,Rong Chen
In this study, nanosized ordered magnetic mesoporous Fe-Ce bimetal oxides (Nanosized-MMIC) with highly well-ordered inner-connected mesostructure were successfully synthesized through the KIT-6 template method. This Nanosized-MMIC displayed excellent adsorption capacities for As(V), Cr(VI) and AO7, and the corresponding calculated maximum adsorption capacities of material were 111.17, 125.28 and 156.52 mg/g, respectively. As(V) and Cr(VI) removal by Nanosized-MMIC were slightly dependent on the ionic strength but highly solution pH-dependent, the coexistent silicate and phosphate ions competed remarkably with both As(V) and Cr(VI) for the adsorption active site. Mechanisms indicated As(V) and Cr(VI) formed inner-sphere complexes on Nanosized-MMIC interface via the electrostatic interaction and surface complexation, while the total organic carbon (TOC) change demonstrated that AO7 could be removed completely and no organic intermediates formed through the adsorption process. In addition, Nanosized-MMIC also possessed superior adsorption performance in As(V)/Cr(VI)-AO7 binary systems, and the reusable and regeneration properties indicated that the obtained nanomaterials could maintain at a comparatively high level after several recycling. Finally, fixed-bed experiments suggested the Nanosized-MMIC was expected to have a promising excellent nano-adsorbent with high application potential for co-existed toxic heavy metals and organic dyes removal in practical wastewater treatment .
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高影响因子
FUEL
·
2025
·
IF 7.5
Jianping Ding,Xiaoyan Zhou,Zhengzheng Yang,Changgeng Liu,Mingchao Sun,Congling Yang,Lu Fan
In this study, a novel strategy was proposed for synthesizing dual single-atom Ce-Ti catalysts supported on γ-Fe 2 O 3 via ball milling and calcination. Compared to γ-Fe 2 O 3 and single-atom Ce/γ-Fe 2 O 3 and Ti/γ-Fe 2 O 3 catalysts, the Ce-Ti/γ-Fe 2 O 3 catalyst exhibits superior NO conversion rates and significantly enhanced tolerance to H 2 O and SO 2 at 200–240 °C. These advancements are attributed to the synergistic interactions between Ce and Ti, which enhance redox properties, increase Lewis acid site density, and facilitate the Langmuir-Hinshelwood reaction pathway. In-situ DRIFTS and density functional theory (DFT) analyses revealed the mechanistic role of surface-active oxygen species and intermediate formation in promoting the SCR reaction. The findings provide valuable mechanistic insights and establish a scalable approach for the development of high-performance, environmentally friendly catalysts for industrial NO x removal.
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CRYSTAL GROWTH & DESIGN
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2024
·
IF 3.2
Pengju Xia,Yifeng Lei,Wanyuan Li,Kaiting Wu,Chengyu Ni,Man Xu,Wubin Dai
With the growing public awareness of protecting vision and prevention of hazardous effects, there is much-needed research on a “healthy” full visible spectrum under near-ultraviolet (nUV) excitation in phosphor-converted white light-emitting diodes (pc-wLEDs) to fill the “cyan gap” and avoid employing a blue LED chip. Herein, a novel series of borosilicates Ba2CaB2Si4O14 (BCBS): Ce3+/Tb3+/Sm3+/Sr2+/Na+ phosphors, presenting color-tunable photoluminescence (PL), high quantum yield (QY), and thermal stability, were designed and synthesized via a facile solid-phase reaction. The Rietveld analyses, density functional theory (DFT) simulations, and theoretical calculations of bond energy together imply the site occupations of Ce/Tb/Sm on Ba2+/Ca2+ sites with a preferred location on Ca2+ over the Ba2+ site. The broad/bright cyan-PL from BCBS: Ce under nUV excitation is associated with the allowed f–d transitions of Ce3+ and dual-site occupancies. The forbidden f–f transitions of both the green-PL of Tb and the red-PL of Sm were insensitive to the site environment and helpful to PL color regulation. The cascading Ce → Tb → Sm energy transfer is confirmed, where Tb is regarded as an energy transfer (ET) bridge to avoid the metal–metal charge transfer (MMCT) effect. The introduction of Na+ as both flux and charge compensator is for the sake of decreasing defects from heterovalent substitutions and regulating morphology. Further incorporation of Sr2+ is to modulate the lattice environments of dopants for controlling the shift of PL. Finally, as a proof-of-concept implement, a pc-wLED assembled by BCBS: Ce/Tb/Sm/Sr/Na and an nUV LED chip via a remote “capping” packaging strategy show attractive performance.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2024
·
IF 5.8
Bin Zhang,Ya’nan Li,Shuai Lu,Jonathan Richard Ishengoma,Song Wang,Jie Liu,Tao Tang,Sanxi Li
Plastic waste causes serious pollution to the environment. Being not satisfied with simply disposing of them into environment, people want to efficiently convert it into high-value products, such as H 2 and carbon nanotubes . A trimetallic catalyst is provided herein, which adds Pr, Ce, La or Yb to a Co-Fe bimetallic catalyst to inhibit the formation of oil by-product in a plastic pyrolysis reaction. In this work,various plastics，including plastics with different functional groups and real plastic waste were used for pyrolysis with elemental hydrogen efficiencies above 95% in the gas product. For pyrolysis of EVA, the gaseous hydrogen efficiency reached 96.07%, and for pyrolysis of LLDPE , the gaseous hydrogen efficiency reached 95.56%, over Pr 1 Co 1 Fe 8 O x catalyst. The role of Pr in catalytic reactions is discussed in general and the formation of carbon nanotubes of various types of structures is simulated. Catalyst cycling experiments demonstrate that the catalyst still maintains a gas hydrogen efficiency of more than 70% after being used four times. In conclusion, the Pr 1 Co 1 Fe 8 O x catalyst proved to be the best choice for microwave-assisted catalytic pyrolysis of plastics to H 2 , and this work provides a new perspect for the study of plastic pyrolysis.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Fajie Hu,Danfeng Zhao,Rushuo Li,Yunqi Zhang,Tianyu Zhang,Xiubing Huang,Ge Wang
The hierarchical porous and chemical microenvironmental properties of Metal–Organic Frameworks (MOFs) have been emphasized in catalytic applications. In this work, after selectively removing ligands from frameworks of Ce-UiO-66 by monocarboxylic acid etching, they exhibit obvious mesoporous properties with essentially unchanged crystallinity. Distinguishing from other pore-making methods, the MOFs have abundant missing sites after etching, and Ni nanoparticles (NPs) can be efficiently anchored in the framework of defective Ce-UiO-66, resulting in the formation of Ce–O–Ni heterogeneous interfaces. The chemical environments of Ni NPs can be modulated through the Ce–O–Ni interfaces, and the metal–support interaction improves the charge densities between the active sites. The prepared catalysts showed high conversion and selectivity in the hydrogenation reaction of dicyclopentadiene, and also had good cycling performance. The present work provides new insights into the construction of hierarchical porous defective MOFs with abundant heterogeneous interfaces for hydrogenation reactions.
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MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Qingmei Qiao,Yunlan Xu,Dengjie Zhong,Xihong Ke,Yuqin Yang,Hanlu Zeng
In order to enhance the carrier separation efficiency and redox ability of photoanode, a dual Z-scheme heterojunction Ce-UiO-66/g-C 3 N 4 /Bi 2 WO 6 /Ti photoanode was prepared and assembled with Cu cathode to form PFC. The characterization results show that Ce-UiO-66/g-C 3 N 4 /Bi 2 WO 6 uniformly distributed on the Ti substrate, with average crystallite size of 9.04 nm and average particle size of 33.05 nm, which provides sufficient reactive active sites for RhB degradation. The RhB degradation rate, P max , J sc , V oc and FF of the PFC were 90.9 % (90 min), 7.53 µW cm -2 , 0.152 mA cm -2 , 0.37 V and 0.134, respectively. The turnover frequency (TOF) for RhB degradation by the PFC reached 0.98 h -1 . Fermi energy level analysis shows that a double-Z heterojunction is formed between Bi 2 WO 6 and g-C 3 N 4 , and between Bi 2 WO 6 and Ce-UiO-66, which not only effectively separates photogenerated e - - h + , but also retains the high redox ability of the composite. Moreover, with the introduction of Ce-UiO-66, the composite photoanode has larger specific surface area and wider visible light absorption range. In addition, because of the built-in electric field, the photogenerated electrons can migrate to the surface of composite particles more easily and react with dissolved oxygen to generate more •O 2 - to participate in the degradation of RhB. This work provides a valuable reference for developing PFC photoanode with high efficiency and visible light response.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Naichuan Yu,Xianhong Zeng,Xingning Ma,Yu Sun,Yixuan Wang,Bingbing Chen,Zhaoqi Luo,Chaofang Dong,Kun Shen,Junsheng Wu
Treating real electroplating wastewater is challenging due to the coexistence of organic contaminants and heavy metal ions, which collectively increase toxicity and pose serious risks to human and environmental health. In this study, the simultaneous removal of a typical organic pollutant (benzodiacetone) and a heavy metal ion (Cr(VI)) from electroplating effluent was investigated using a heterogeneous electro-Fenton process catalyzed by a novel Ce-Fe 2 O 3 /Al 2 O 3 material. Comprehensive characterization and theoretical calculations confirmed the excellent catalytic performance of the synthesized catalyst. Under near-neutral conditions, the electro-Fenton system achieved removal efficiencies of 99.1 % for benzodiacetone and 98.8 % for Cr(VI). The mechanism of simultaneous degradation was explored, revealing that Ce doping enhanced Fe redox cycling by lowering the binding energy between H 2 O 2 and Fe and facilitating electron transfer from Fe (III) to Fe (II). Additionally, Ce doping improved the stability and reusability of the catalyst. And the Ce could also extend the lifetime and reusability of the catalyst. This work developed a highly efficient heterogeneous catalyst in the electro-Fenton process and demonstrated that the Ce-Fe 2 O 3 /Al 2 O 3 catalyst had a superior application potential in synergic removal of Cr(VI) and benzodiacetone area.
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