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RSC Advances · 2017 ·Vol. 7 ·期 14 ·8567-8574 · IF 3.108

Effect of tungsten surface density of WO3–ZrO2 on its catalytic performance in hydrogenolysis of cellulose to ethylene glycol

Jiachun Chai,Shanhui Zhu,Youliang Cen,Jing Guo,Jianguo Wang,Weibin Fan

One-pot hydrogenolysis of cellulose to ethylene glycol (EG) was carried out on WO3-based catalysts combined with Ru/C. To probe the active catalytic site for breaking the C–C bond of cellulose, a series of WO3–ZrO2 (WZr) catalysts were synthesized and systematically characterized with XRD, Raman, UV-Vis, H2-TPR, DRIFS and XPS techniques and N2 physisorption experiment. It was found that the WO3 crystallites became more easily reduced to W5+–OH species with increasing crystallite size or tungsten surface density of the WZr catalyst owing to the decrease of their absorption edge energy (AEE) originating from weakening their interaction with ZrO2 support. This, as a result, gave higher EG yield at higher tungsten surface density. The structure–activity relationship of the WZr catalyst reveals that the active catalytic site for cleaving the C2–C3 bond of the glucose molecule is the W5+–OH species.

CAS / MDL: 14475-63-9 7440-18-8
研究领域: 催化化学 · 材料科学
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Journal of Energy Storage · 2023 · IF 9.4

Free-standing graphene/polyetherimide/ZrO2 porous interlayer to enhance lithium-ion transport and polysulfide interception for lithium-sulfur batteries

Jiuqing Liu,Fanli Zeng,Zikun Hong,Junying He,Qihou Li,Feifei Song,Lishun Bai,Chen Cheng,Zehao Chen,Liandong Tang,Chen Duan,Zhirong Chen

Attributing to high theoretical specific capacity and energy density , lithium-sulfur batteries (LSBs) are receiving great attention. However, the commercialization of such technology is seriously hindered by the shuttle effect of polysulfides during the round-trip charge and discharge process. Herein, with three types of carbon materials and ZrO 2 nanoparticles filled in polyetherimide (PEI) support framework with good stability, porous composite films were obtained by a simple non-solvent phase separation (NIPS) as free-standing interlayers for LSBs. The obtained interlayers can not only provide hierarchical channels for improving lithium-ion transfer number, but also own excellent physicochemical stability and strong adsorption capability towards lithium polysulfide (LiPS). Compared with the pristine one, the representative LSB with graphene/polyetherimide/ZrO 2 interlayer (GPZ) shows good initial cycle discharge specific capacity (1280 mAh g −1 ), better capacity retention (749 mAh g −1 after 200 cycles) and good rate performance (580 mAh g −1 at 2C). This work provides a facile and promising way to achieve functional interlayer with high stability for high performance LSBs.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF NANOPARTICLE RESEARCH · 2018 ·Vol. 20 ·期 6 ·1-13 · IF 2.127

A composite material with CeO2-ZrO2 nanocrystallines embedded in SiO2 matrices and its enhanced thermal stability and oxygen storage capacity

Yang Runnong,Liu Yumei,Yu Lin,Zhao Xiangyun,Yang Xiaobo,Sun Ming,Luo Junyin,Fan Qun,Xiao Jianming,Zhao Yuzhong

A simple hydrothermal procedure is introduced, which leads to the successful synthesis of a new composite material with fine CeO 2 -ZrO 2 nanocrystallites embedded in amorphous and porous SiO 2 matrices. The composite material possesses an extraordinary high thermal stability. After being calcined at 1000 °C, it retains CeO 2 -ZrO 2 nanocrystallites of the size around 5 nm, a BET-specific surface area of 165 m 2 /g, and an oxygen storage capacity of 468 μmol/g. No phase segregation for CeO 2 -ZrO 2 nanocrystallites is detected and the SiO 2 matrices remain not crystallized. The composite material shows a great potential as a support of three-way catalyst, as evidenced in catalytic tests with supported Pt.

研究领域: 材料科学 · 催化化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2014 · IF 6.007

Combining HC-SCR over Ag/Al2O3 and hydrogen generation over Rh/CeO2-ZrO2 using biofuels: An integrated system approach for real applications

Fredrik Gunnarsson,Moa Z. Granlund,Mattias Englund,Jazaer Dawody,Lars J. Pettersson,Hanna Härelind

We report on a high NO x reduction activity over Ag/Al 2 O 3 catalysts, using hydrogen produced in a fuel reformer. The focus of the study is to evaluate the performance of a hydrocarbon selective catalytic reduction (HC-SCR) catalyst in real conditions. Initially, the catalytic materials for the fuel reformer (Rh/CeO 2 -ZrO 2 ) and the HC-SCR (Ag/Al 2 O 3 ) were evaluated in separate bench-scale reactor setups. These two setups were subsequently joined into an integrated bench-scale reactor setup with the aim to evaluate the influence of the reformate on the HC-SCR activity in a controlled environment. In the final phase of the study a 4   wt.% Ag/Al 2 O 3 catalyst doped with 100   ppm(w) Pt was scaled up and tested in a pilot-scale reactor setup. The pilot-scale reactor setup enabled evaluation of the HC-SCR activity in real exhaust gases generated by a single cylinder engine (genset) together with a hydrogen-rich gas supplied from a fuel reformer. Commercial biodiesel (NExBTL) was used as reducing agent for the HC-SCR as well as fuel in the fuel reformer for both the bench-scale and pilot-scale experiments. This study gives an excellent link between evaluations of the catalytic materials, controlled bench-scale experiments and applied engine experiments, proving a viable concept for lean NO x reduction together with onboard hydrogen production. A NO x conversion of above 70% was reached at temperatures below 250   °C, in bench-scale experiments when hydrogen produced in the fuel reformer is added.

研究领域: 环境科学 · 催化化学 · 能源工程
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Highly Selective Conversion of Furfural to Furfural Alcohol or Levulinate Ester in One Pot over ZrO2@SBA-15 and Its Kinetic Behavior

Junhua Zhang,Yao Liu,Shibo Yang,Junnan Wei,Liang He,Lincai Peng,Xing Tang,Yonghao Ni

Biorefinery for the purpose of producing biofuels, chemicals, and materials has received much attention. Furfural alcohol (FOL) and levulinate ester (LE) are important biomass-derived platform chemicals, and they are produced from sugar-based furfural (FAL). Unfortunately, the two products are often obtained separately in different reaction systems, which is undesirable; furthermore, it is of significant practical interest to control their selectivity so that the desired product can be accumulated in high yields. Herein, we present an efficient method for the highly selective conversion of FAL to FOL or isopropyl levulinate (IPL) in a one pot system using isopropanol as the hydrogen source and ZrO2@SBA-15 as a bifunctional catalyst with both Lewis acid and Brønsted acid sites. Under optimized reaction conditions, high yields of FOL and IPL in up to 90.4% and 87.2%, respectively, were obtained. Based on the experimental results, a kinetic model describing the catalytic conversion of FAL into FOL and IPL process has been established, which has a good correlation (R2 > 0.92) between the measured and predicted data. The developed kinetics can provide an effective tool to monitor the process and tailor the process conditions to obtain the desired product.

CAS / MDL: 7789-75-5 59-30-3
研究领域: 生物炼制 · 催化化学 · 绿色化学
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ChemSusChem · 2022 ·Vol. 15 ·期 13 ·e202200092 · IF 9.14

Selective Hydrogenolysis of 5-Hydroxymethylfurfural to 2-Hexanol over Au/ZrO2 Catalysts

Xiaohong Hu,Zhijian Li,Haiyong Wang,Haosheng Xin,Song Li,Chenguang Wang,Longlong Ma,Qiying Liu

Graphical Ring-opening : Au/ZrO 2 catalysts with excellent ring-opening hydrogenolysis ability are developed for the selective hydrogenolysis of 5-hydroxymethylfurfural and furfural to produce 2-hexanol and pentanol (1-pentanol and 2-pentanol). The Au-O−Zr interfaces with Lewis acid and metal functionalities play key roles for obtaining the target products with high yield. 2-Hexanol (2-HOL) is a versatile biomass-derived platform molecule for synthesis of liquid transportation fuels, lubricants, or detergents. Herein, a one-step preparation of 2-HOL using 5-hydroxymethylfurfural (HMF) as a substrate was reported for the first time. Several Au-based catalysts supported on different metal oxides were prepared to explore the relationship between carrier and catalytic activity. The results showed that the highest 2-HOL yield of 65.8 % was obtained at complete HMF conversion over the 5 %Au/ZrO 2 catalyst. The 5 %Au/ZrO 2 catalyst exhibited excellent durability after five consecutive recycling runs, while confirming its remarkable ring-opening hydrogenolysis on other biomass-derived furanics, furfural, with a total yield of 1-pentanol and 2-pentanol of 67.4 %. The distinguished ring-opening hydrogenolysis performance of the Au/ZrO 2 catalyst originated from a synergistic effect between the interfacial Au-O-Zr oxygen vacancies-induced Lewis acidic sites (activating C−OH/C=O bonds) and metallic Au (activating H 2 ). This work provides a possibility for producing 2-HOL from HMF with high yield, expanding the sustainable application of lignocellulosic biomass.

研究领域: 催化 · 化学工程 · 可再生能源 · 绿色化学
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BIOMASS & BIOENERGY · 2022 · IF 5.774

Insight into the selective production of aldehydes and ketones by catalytic upgrading of biomass pyrolysis vapor over ZrO2:Cellulose and xylan

Shanshan Shao,Chengyue Liu,Xianliang Xiang,Xiaohua Li,Huiyan Zhang,Rui Xiao

Catalytic upgrading of pyrolysis gas components from cellulose and xylan was investigated over ZrO 2 catalyst to produce aldehydes and ketones . The oxygen content in the bio-oil was reduced by aldol condensation and hydrogenation of aldehydes and ketones. The optimal pyrolysis temperature of cellulose and xylan were determined to be 400 °C and 350 °C and the carbon yields of aldehydes and ketones reached 54.49% and 52.05% respectively. In order to explore the formation mechanism of aldehydes and ketones, the evolution of typical products by controlling the reaction time was studied. The catalytic pyrolysis was complete and the product content was maximum at 20 min H 2 O played a role in providing oxygen atoms and increasing ZrO 2 reaction activity in the carbonylation process. The binding energy of the catalyst was calculated as −15.69 kcal/mol by density functional theory (DFT). It was found that the presence of water can remove the coke on the catalyst surface and increase the activity of ZrO 2 . The yield of aldehydes and ketones reached 58.17% and 55.85% of cellulose and xylan with the presence of 15 wt% H 2 O in the carbonylation process. According to the evolution of the above experimental products, the generation pathways of four main carbonylation products (acetone, methyl ethyl ketone , butyraldehyde and furfural) were proposed. Through this research, the effective utilization of biomass could be realized.

研究领域: 能源与环境科学 · 催化化学
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JOURNAL OF POROUS MATERIALS · 2019 ·Vol. 27 ·期 2 ·429-440 · IF 1.947

Preparation, characterization, and application of ordered mesoporous S2O82−/ZrO2–SiO2 with high specific surface area

Wang Yunjie,Yuan Hong,Zhang Zhi,Ke Yihu

A series of ordered mesoporous S 2 O 8 2−/ ZrO 2 –SiO 2 (OMSZS) solid superacids with different calcination temperatures (400–650 °C) was synthesized using zirconium n-propoxide and tetraethyl orthosilicate as the raw materials and P123 as a structure-directing agent by solvent evaporation-post-dipping method. Transmission electron microscopy and small-angle X-ray diffraction results showed that the OMSZS were all ordered. The nitrogen adsorption results indicated that the specific surface area of OMSZS could reach up to 331–385 m 2 /g, whereas the average pore diameters were in the range of 3.1–3.2 nm. The pyridine infrared results mainly displayed Lewis acids, and the ammonia (NH 3 )-temperature programmed desorption characterization showed that the NH 3 desorption of the OMSZS calcined at 550 °C was 61 cm 3 /g STP. The catalytic performance of the OMSZS was investigated by the transesterification reaction of waste frying oil and methanol. The yield of fatty acid methyl ester could reach up to 94% at 200 °C reaction temperature for 6 h. After repeated use for four times, the catalyst still featured good activity and the yield was 78%.

研究领域: 材料科学 · 催化化学
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MATERIALS CHARACTERIZATION · 2022 · IF 4.537

Structure and fracture behavior of ion-beam-modified SiC-Al2O3-ZrO2 ceramic composites

Jianlong Chai,Yabin Zhu,Peng Jin,Tielong Shen,Lijuan Niu,Shufen Li,Minghuan Cui,Zhiguang Wang

SiC-Al 2 O 3 -ZrO 2 ceramic composite with heterointerfaces was prepared by hot pressing and irradiated with 1.2 MeV Si ions at room temperatures. The microstructural evolution and mechanical properties were investigated. The results showed that the phase transformation of zirconia revealed by GIXRD and TEM are associated with the accumulation of oxygen vacancies clusters originated by damage and the size of displacement cascades. Complete amorphization of SiC particles were observed at 5.5 dpa, and developed into collection band at 55 dpa due to the mixture of point defect clusters and extend defects at high damage level. The nanohardness and elastic modulus irradiation decreased with increasing of damage level. The fracture behavior of materials and relative mechanism under ion irradiation were discussed.

研究领域: 材料科学 · 核材料工程
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Preparation of MoSi2@ZrO2 core-shell powders by hydrothermal-calcination and evaluation of low-temperature oxidation resistance

Ciwang Quan,Xianjun Yang,Jiajun Luo,Ziqiao Wang,Yushuai Feng,Jianjun Zhang,Weihua Chen,Bingliang Liang

MoSi 2 is a promising candidate for high-temperature, structural materials. However, their oxidation resistance is poor below 600 °C. To prevent MoSi 2 from being oxidized at low temperatures, core-shell structured MoSi 2 @ZrO 2 powder were prepared by hydrothermal-calcination approach. First, MoSi 2 @Zr(OH) 4 core-shell composite powder with nano-sized Zr(OH) 4 shell particles were synthesised using a hydrothermal method . Subsequently, the MoSi 2 @ZrO 2 core-shell structured powder were obtained by calcination of the MoSi 2 @Zr(OH) 4 powders at 900 °C for 2h. Finally, microstructure and oxidation behaviour of the MoSi 2 @ZrO 2 powder at 400 °C–600 °C in air were investigated systematically. Microstructural analysis revealed that all samples had a distinct core-shell structure, and the ZrO 2 shells coated the surface of the MoSi 2 core. Oxidation behaviour studies showed that the dense ZrO 2 shell layer could isolate the MoSi 2 surface from oxygen, improving the low-temperature oxidation resistance and providing better low-temperature antioxidant properties than those of the MoSi 2 and MoSi 2 @Zr(OH) 4 core-shell structures.

CAS / MDL: 13520-92-8
研究领域: 材料科学 · 高温材料 · 氧化行为研究
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RSC Advances · 2017 ·Vol. 7 ·期 14 ·8709-8717 · IF 3.108

Structure–activity relationships of Cu–ZrO2 catalysts for CO2 hydrogenation to methanol: interaction effects and reaction mechanism

Yu Hao Wang,Wen Gui Gao,Hua Wang,Yan E. Zheng,Wei Na,Kong Zhai Li

A series of Cu–ZrO2 (CZ) catalysts with different surface area, copper surface area (SCu), oxygen vacancy concentration, and interaction between Cu and ZrO2 features were synthesized. The factors that could affect catalytic activity of CO2 hydrogenation to methanol were investigated. The interaction between Cu and ZrO2 is crucial for determining the catalytic activity. The catalyst possessing the strongest interaction between Cu and ZrO2, exhibited the optimum catalytic activity. The evolution of carbonaceous species and pyridine adsorption over CZ catalysts were investigated using in situ DRIFT spectroscopy. It is found that the hydrogenation of formate species is a rate-limiting step and H spillover plays an important role. The hydrogenation of formate species and H spillover are strongly dependent on the interaction. These results provide a new way of understanding the activity dependence and reaction mechanism of CO2 hydrogenation to methanol over CZ catalysts.

CAS / MDL: 10031-43-3
研究领域: 催化化学 · 能源化学
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TRIBOLOGY INTERNATIONAL · 2023 · IF 6.2

Improving the tribological properties of ZrO2(Y2O3)-graphite composites at high temperature through three-dimensional continuous structure

Pengyu Lin,Junjie Song,Xin You,Qiuan Sun,Tao Li,Jiaxin Si,Haifeng Wang,Litian Hu,Yongsheng Zhang

ZrO 2 (Y 2 O 3 )-graphite composites with a three-dimensional (3D) continuous structure were prepared by using a core-shell design of graphite and ZrO 2 (Y 2 O 3 ). The effect of structure on the friction-reducing and anti-wear mechanisms from room temperature to 700 °C was investigated. During high-temperature friction, abrasive wear and brittle fracture are the main wear mechanisms for ZrO 2 (Y 2 O 3 )-graphite composites with homogeneous composition. For the composites with 3D structure, the continuous ZrO 2 matrix with high load-carrying capacity and the formation of a dense friction layer with self-lubricating and thermal oxidation resistance improve the tribological properties significantly, reducing the coefficient of friction by about 10% and the wear rate by nearly two orders of magnitude when coupled with GH4169 alloys at 600 °C.

CAS / MDL: 7782-42-5
研究领域: 材料科学 · 摩擦学
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