INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Na Sun,Linlin Xiang,Bingsen Zhuge,Erjie Kan,Nan Yu,Lei Li,Long Kuai
Low-temperature catalytic CO oxidation is an important chemical process in versatile applications, such as the H2 utilization for low-temperature H2 air fuel cells. Pt-group metal catalysts are efficient but highly cost-consuming. This work demonstrates an excellent and sixpenny catalyst with earth-abundant Ni and Ce, in which Ni ions are atomically incorporated into the CeO2 matrix (Ni–Ce–Ox) by synchronous spray-pyrolysis (SSP) of mixture nitrates of Ni and Ce. The Ni–Ce–Ox catalyst presents a mesoporous structure. Revealed by a model reaction of 1% CO, 1% O2, and 98% balance He at a space velocity of 13,200 mL/gcat/h, Ni–Ce–Ox catalysts display a typical volcano-shaped relationship between reactivity and Ni incorporation amount. The optimized Ni incorporation appears with a high Ni/Ce atomic ratio of 0.25, endowing the T50 (temperature corresponding to a CO conversion of 50%), which is lower-shifted by 165 °C than that of pristine CeO2 (266 °C). The density functional theory (DFT) calculations further indicate that the much-reduced oxygen vacancy formation energy at Ni–Ce single-atom sites boosted the adsorption activation of the CO molecule and therefore promoted the CO oxidation process. Besides, the2 Ni–Ce–Ox from the SSP method presents better performance than the counterparts from immersion and hydrothermal methods. This work paves a way to access efficient noble-metal-free catalysts for low-temperature CO oxidation.
研究领域:
催化化学
·
材料科学
·
环境化学
·
能源化学
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表面科学
·
纳米材料
·
计算化学
✓ 已验证
DOI
高影响因子
Small
·
2026
·
IF 11.8
Wuxi Zhang,Jianyu Li,Yangke Cun,Xinmin Bai,Yingzhu Zi,Zan Xu,Jianbei Qiu,Zhaoyu Ma,Junying Zhang,Zhengwen Yang
Most widely-studied semiconductor catalysts have low efficiency in utilizing near-infrared (NIR) light in the solar spectrum, while also facing major issues such as slow charge-carrier migration rate and lack of active sites that limit photocatalytic performance. Here, a new strategy to promote the solar-light driven photocatalytic activity of ZnIn 2 S 4 was proposed by introducing Rh single atom (SAs) into CeO 2 :Yb,Er/ZnIn 2 S 4 with photo-thermo-electric effects. The introduction of Rh SAs into ZnIn 2 S 4 effectively suppresses charge recombination, and improves reaction rate through photo-thermal effect. CeO 2 :Yb, Er converts NIR light into visible light via up-conversion photo-optical processes and generates high-energy electrons via two-photon photo-electronic process, both of which can activate ZnIn 2 S 4 . Large contact area and strong interface electric field between CeO 2 and ZnIn 2 S 4 enhance photo-electric conversion efficiency. The CeO 2 :Yb,Er/Rh-ZnIn 2 S 4 exhibits a hydrogen production rate of up to 99.68 mmol·g −1 ·h −1 at 10°C and 148.06 mmol·g −1 ·h −1 with non-temperature-controlled conditions. Under mild conditions, the photocatalysts can convert glucose into high-value-added chemicals (e.g., arabinose) while simultaneously generating hydrogen. This work provides a new strategy to improve NIR light utilization efficiency and enhance charge-carrier separation capability through photo-thermo-electric effects, promoting the production of green hydrogen and biomass conversion into high-value-added chemicals.
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Shuang Wei,Sheng Zhong,Chao Bao,Linbo Huang,Kexin Li,Ruirui Wang,Bin He,Ruirui Zhang,Ruixia Liu
The selective electrocatalytic oxidation of glycerol to high-value C2–C3 chemicals offers a promising approach to glycerol overproduction, while it struggles with precise C–C cleavage and limited selectivity from multiple pathways. Regulating the adsorption capacity of glycerol oxidation intermediates and the degree of C–C bond cleavage through the interfacial electronic structure of electrocatalysts is crucial for controlling C2–C3 selectivity. Herein, a self-supported p-n heterojunction catalyst (Co3O4/CeO2) is developed for the efficient electrocatalytic oxidation of glycerol to C2 chemicals, achieving a glycolic acid selectivity of 42%, with a yield of 19.6 μmol cm–2 h–1. The built-in electric field enables rapid interfacial charge transfer from CeO2 to Co3O4, which leads to the upshifted d-band center of active Co3O4. Electrochemical characterization and theoretical calculations demonstrate that the heterojunction promotes the adsorption of hydroxyl species and glycerol, thereby enhancing the activity of the glycerol oxidation reaction (GOR). Concurrently, the optimized electron cloud distribution of Co3O4 active sites strengthens the adsorption of oxygen-containing intermediates while weakening the adsorption of glycolic acid and suppresses the further cleavage of C–C bonds, thus increasing glycolic acid selectivity. This study clarifies the redox kinetic adsorption regulation mechanism of the Co3O4/CeO2 heterojunction catalyst and provides a highly promising electrocatalyst design strategy for the production of high-value-added C2 products via glycerol oxidation.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Cui Lai,Fuhang Xu,Mingming Zhang,Bisheng Li,Shiyu Liu,Huan Yi,Ling Li,Lei Qin,Xigui Liu,Yukui Fu,Ning An,Hailan Yang,Xiuqin Huo,Xiaofeng Yang,Huchuan Yan
CeO 2 nanoparticles are successfully loaded on carbonate doped Bi 2 O 2 CO 3 (CBOC) nanosheets by a facile hydrothermal and low-temperature calcination method. CeO 2 /CBOC heterojunction shows significantly enhanced photocatalytic activity, when 35 mg of CeO 2 /CBOC photocatalyst is added to tetracycline (TC) solution (20 mg/L, 100 mL), about 79.5% TC is degraded within 90 min under visible light irradiation, which is much higher than that of original CeO 2 and CBOC. According to photoelectrochemical characterization and active radical capture experiments, the Z-scheme electron transfer mechanism is the reason for the significant enhancement of photocatalytic activity . Besides, the XPS results indicate that Ce 4+ /Ce 3+ redox pairs are formed at the contact interface between CeO 2 and CBOC, which is conducive to the transfer of photoexcited electrons and production of superoxide radicals. Additionally, the photocatalytic mechanism and possible degradation pathway of TC is proposed through free radical trapping experiments and liquid chromatography-mass (LC-MS) analysis. This study will accumulate experience for the combination of CeO 2 and bismuth-based nanomaterials , and provide a feasible way to design wide band-gap bismuth-based photocatalysts, thereby achieving efficient visible light degradation of environmental pollutants .
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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2014
·
IF 3.309
Yuxi Gao,Xiaodong Wu,Shuang Liu,Duan Weng,Hongwei Zhang,Rui Ran
MnO x –CeO 2 mixed oxides were synthesized using a sol–gel method and the barium-loaded catalyst was prepared by a wet impregnation. Both catalysts were hydrothermally aged at 800 °C for 10 h. The fresh and aged catalysts were characterized by X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), high-resolution transmission electron microscopy (HRTEM), H 2 temperature-programmed reduction (H 2 -TPR), NO temperature-programmed oxidation (NO-TPO) and soot temperature-programmed oxidation (soot-TPO). Compared with MnO x –CeO 2 , the Ba-modified mixed oxides show a much higher hydrothermal stability. Barium exists in the form of orthorhombic carbonate and cubic nitrate on the fresh sample. BaMnO 3 nanoparticles are identified to form at the interface of CeO 2 crystallites upon the hydrothermal ageing. The formation of the perovskites prohibits the sintering of ceria significantly, and consequently maintains the redox property of the aged mixed oxides to a great degree. Additionally, the nanoscaled perovskites themselves also contribute to the catalytic activity of the aged oxides catalyst.
研究领域:
催化材料
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hao Li,Qin-Hao Zhang,Xian-Ze Meng,Hao-Jie Yan,Hui-Song Hu,Lian-Kui Wu,Fa-He Cao
In the marine environment, besides external damage and internal defects, ultraviolet (UV) radiation is also a pivotal factor affecting the stable properties of coatings. Improving the anti-UV aging and active protection properties is beneficial to prolong the service life of coatings. Herein, the PDA-GO-CeO 2 composite material is obtained through a facile stepwise growth of polydopamine (PDA) and CeO 2 on GO nanosheets and further preparing a multifunctional anti-corrosion PDA-GO-CeO 2 -EP coating. As expected, composite coating displays strong adhesion force (6.9 MPa) and tensile strength (21.1 MPa), profiting from the enhanced crosslinking density and interface structure caused by PDA-GO-CeO 2 and resin matrix interaction. Since low defect functionalized PDA-GO-CeO 2 constructs the reinforced physical barrier, the anti-corrosion ability of PDA-GO-CeO 2 -EP coating (10 9.7 Ω·cm 2 ) is more dependable than those of EP (10 6.7 Ω·cm 2 ), GO-EP coating (10 8.8 Ω·cm 2 ) and PDA-GO-EP (10 9.1 Ω·cm 2 ) coatings after immersing in 3.5 wt.% NaCl solution for 100 d. Thanks to the synergistic effect of PDA/CeO 2 , the active protection performance of PDA-GO-CeO 2 -EP coating is endowed, which is further proved through the in situ scanning vibrating electrode technique (SVET). Following the UV aging treatment, PDA-GO-CeO 2 -EP coating shows minor gloss loss (20.4 %) and better adhesion force (4.3 MPa). Furthermore, the resistance value of PDA-GO-CeO 2 -EP coating is 7.03 × 10 6 Ω cm 2 after 30 d immersion in saline solution, which is 242 times greater than that of EP coating (2.90 × 10 4 Ω cm 2 ). This dependable performance of PDA-GO-CeO 2 -EP coating comes from the reflection, refraction, and absorption of UV rays by nanoscale CeO 2 particles. Consequently, this work offers a simple and promising strategy for fabricating multifunctional long-term protection coatings, thus hopefully extending the service life of marine engineering equipment.
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产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2023
·Vol. 40
·期 12
·3059-3067
·
IF 2.7
Yin Zihang,He Ruibo,Nie Fei,Wei Zhen,Jia Bo,Feng Qing,Fu Xiaolong,Zhang Wenyan
The oxygen evolution kinetics of industrial copper electrodeposition is slow, resulting in low electrocatalytic activity and high energy consumption. In this work, a quaternary composite of carbon coated active particles containing Mn, Co and Ce were prepared (Mn-Co 3 O 4 /CeO 2 @C), and Ti/Sb-SnO 2 /PbO 2 electrode doped with these active particles was prepared by co-electrodeposition. The microstructure and chemical composition of the electrode was characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and X-ray diffractometry (XRD). Linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS) and Tafel polarization curve (Tafel) were used to study the electrochemical properties of anode materials. The results showed that the doping of Mn-Co 3 O 4 /CeO 2 @C active particles promoted the crystal transition of PbO 2 , decreased the average grain size, and the doping of Ce increases the average valence state of Co. The modified titanium electrode showed excellent catalytic activity of the oxygen evolution reaction (OER) characteristics. The overpotential of the doped Ti/Sb-SnO 2 /PbO 2 anode was only 453 mV when the current density was 20 mA cm −2 in 0.5 M H 2 SO 4 solution, which is 508 mV lower than that of the undoped Ti/Sb-SnO 2 /PbO 2 anode. In simulated copper electro-deposition experiments, the cell voltage was reduced by about 400 mV, compared to the undoped Ti/Sb-SnO 2 /PbO 2 electrode.
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产品关联
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Bo Yuan,Zicong Tan,Qiang Guo,Xiutong Shen,Chao Zhao,Jian Lin Chen,Yung-Kang Peng
Nanozymes are promising alternatives to natural enzymes, but their use remains limited owing to poor specificity. For example, CeO2 activates H2O2 and displays peroxidase (POD)-like, catalase (CAT)-like, and haloperoxidase (HPO)-like activities. Since they unavoidably compete for H2O2, affecting its utilization in the target application, the precise manipulation of reaction specificity is thus imperative. Herein, we showed that one can simply achieve this by manipulating the H2O2 activation pathway on pristine CeO2 in well-defined shapes. This is because the coordination and electronic structures of Ce sites vary with CeO2 surfaces, wherein the (100) and (111) surfaces display nearly 100% specificity toward POD-/CAT-like and HPO-like activities, respectively. The antibacterial results suggest that the latter surface can well-utilize H2O2 to kill bacteria (cf., the former), which is promising for anti-biofouling applications. This work provides atomic insights into the synthesis of nanozymes with improved activity, reaction specificity, and H2O2 utilization.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Zuozhu Yin,Zihao Li,Yuanting Deng,Mingshan Xue,Yuhua Chen,Junfei Ou,Yu Xie,Yidan Luo,Chan Xie,Zhen Hong
Complicated contaminants in wastewater, such as intractable oils, organic colors, and adhering organisms, have generated major environmental problems that are hazardous to ecosystems and human health, and wastewater purification is complex and difficult to achieve with a single substance or single process. A facile yet environmentally friendly technique for fabricating a superhydrophobic, oil-water separation, anti-bioadhesion, and photocatalytic Pulp/cellulose nanofibers (CNFs) membrane for all-in-one wastewater treatment is presented here. In this strategy, the hierarchical micro/nanostructured CeO 2 nanoparticles and stearic acid (STA)-coated Pulp/CNF (Pulp/CNF-CeO 2 -STA) membrane is fabricated via a straightforward and easy-to-operate coating method, which simultaneously endows the membrane with superwetting ability, good oil-water separation capacity, notable photocatalytic degradation capacity, and outstanding anti-bioadhesion action. According to the experimental results, the suitably prepared Pulp/CNF-CeO 2 -STA membrane displayed superior superhydrophobicity (water contact angle: 166 ± 2°), high separation efficiency (88%), and high throughput (73 L·m −2 ·h −1 ). This Pulp/CNF-CeO 2 -STA membrane also showed significant photocatalytic degradation (>94%) of organic dye pollutants in water, as well as good anti-bioadhesive performance against Chlorella . As such, it serves several functions in wastewater treatment, considerably simplifying installation and saving money in application. In conclusion, this unique coating process is environmentally benign and very practicable, paving the door for the development of multi-functional materials in environmental treatments.
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Jingyang Luo,Wangbei Cao,Wen Guo,Shiyu Fang,Wenxuan Huang,Feng Wang,Xiaoshi Cheng,Wei Du,Jiashun Cao,Qian Feng,Yang Wu
Various pollutants commonly co-exist in the waste active sludge (WAS), but the interactive effects and mechanisms of co-occurrence pollutants on the WAS treatment remain unclear. This work mainly investigated the impacts of different surfactants ( i.e., HTAB and SDBS) and CeO 2 nanoparticles (NPs) co-occurrence on the WAS fermentation for short-chain fatty acids (SCFAs) production, and found that the CeO 2 NPs coexisting with surfactants caused antagonistic effects on the SCFAs generation (10.7% and 33.9% inhibition by HTAB and SDBS , respectively). The surfactants and CeO 2 NPs co-occurrence restrained the solubilization , hydrolysis , and acidification steps simultaneously. Moreover, the functional hydrolytic-acidogenic bacterial ( e.g., Haliangium and Bacteroidetes sp. ) and the microbial metabolic networks involved in extracellular hydrolysis ( e.g., pepd and NEU1 ), substrate metabolism ( e.g., ALDO and asdA ), and fatty acid biosynthesis ( e.g. , aarC and pct ) were all downregulated by 4.3–53.8% in the reactors with surfactants and CeO 2 NPs co-occurrence. The presence of surfactants enhanced the dispersibility and stability of CeO 2 NPs and the Ce dissolution (1.5–3.0 times higher). Also, surfactants contributed to the WAS disintegration, which could improve the interactive chances of microorganisms entrapped in WAS and CeO 2 NPs by promoting the transportation channels, and therefore aggravated the toxicity towards anaerobic species.
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产品关联
DOI
PubMed
高影响因子
Materials
·
2023
·Vol. 16
·期 14
·5063
·
IF 3.4
Liu Yang,Yongchang Zhu,Jichuan Huo,Zhu Cui,Xingquan Zhang,Xuanjiang Dong,Jie Feng
Low-alkali borosilicate glass was used as the immobilization substrate, and Ce was used to replicate the trivalent and tetravalent actinides, in order to create simulated waste glass through melt heat treatment. The valence of Ce and solubility of CeO2in waste glass were studied as well as its network structure and thermal and chemical stability. The solubility of Ce in waste glass was examined by XRD and SEM. The network structure was examined by Raman spectroscopy. The valence of Ce was determined by X-ray photoelectron spectroscopy. Thermal analysis and product consistency (PCT) were employed to determine the thermal and chemical stability of waste glasses. The results show that the solubility of cerium in low-alkali borosilicate glasses is at least 25.wt.% and precipitates a spherical CeO2crystalline phase when it exceeds the solid solution limit; Ce is immobilized in the glass by entering the interstices of the glass network. Depolymerization and the transition from [BO3] to [BO4] occurs when CeO2doping levels rise. About 60 percent of Ce4+is converted to Ce3+, and the thermal stability of glass rises then falls with the increase of CeO2. All samples exhibit strong leaching resistance, with the average mass loss of Ce at 28 days being less than 10−4gm−2d−1.Keywords:low-alkali borosilicate;cerium;Raman;XPS
研究领域:
材料科学
·
环境工程
·
核废料管理
·
光谱学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Songlei Mo,Jia Kou,Jianrong Zeng,Kepeng Song,Yayun Zhang,Shangming He,Yongfeng Hu,Yong Guo,Xiaohui Liu,Xi Chen,Yanqin Wang
Upcycling polyethylene terephthalate (PET) wastes into high value-added oxygenated chemicals is desirable, yet it remains challenging. Herein, we develop a novel strategy to convert PET into 1,4-cyclohexanedimethanol (CHDM) via two steps, the conversion of PET to dimethyl 1,4-cyclohexanedicarboxylate (DMCD) over Ni-based catalysts, followed by the hydrogenolysis of DMCD to CHDM over a CuMgAl catalyst. The key step is the production of DMCD from PET in one-pot reaction and an unprecedent yield of 86.5% DMCD yield is achieved over Pd-modified Ni/CeO 2 catalyst, which to the best of our knowledge is the highest yield reported to date. Comprehensive characterizations demonstrate that the addition of Pd enhances hydrogen dissociation, but weakens the adsorption activation ability for C–O bond in esters, thus DMCD selectivity is improved. Over CuMgAl catalyst, DMCD is directly converted into CHDM with 83.8% yield. Furthermore, the techno-economic analysis proves the economic feasibility of converting PET into CHDM via our proposed strategy. The study provides a promising and effective approach to upcycle PET wastes into high value-added products.
研究领域:
化学工程
·
催化
·
废物管理
·
可持续化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）