RENEWABLE ENERGY
·
2019
·
IF 5.439
Qing Zhou,Xinyan Zhong,Xingyue Xie,Xuanyi Jia,Baiquan Chen,Ning Wang,Lihong Huang
Biomass-derived acetic acid (HAc), as a hydrogen storage medium, can be transformed to hydrogen via on-board reformer for fuel cells. Steam reforming (SR) of HAc is a traditional hydrogen production process, but endothermicity of SR is a concern for heat management in dynamic on-board application. Auto-thermal reforming (ATR) of HAc is a promising route, while catalyst deactivation in harsh ATR atmosphere should be addressed. Samarium-promoted ordered mesoporous Ni-xSm-Al-O catalysts were synthesized via improved evaporation-induced self-assembly (EISA) method, and tested in ATR of HAc for hydrogen production. The Ni-2Sm-Al-O catalyst produced a stable HAc conversion near 100.0% and a hydrogen yield at 2.6 mol-H 2 /mol-HAc in a 30-h test. Meanwhile, the Ni-2Sm-Al-O catalyst shows resistance to oxidation , sintering and coking; this improved reactivity and durability can be attributed to basic Sm oxides and ordered mesoporous framework with confinement effect : the basic sites are beneficial to adsorption and activation of HAc, and the ordered mesoporous framework constrains the thermal agglutination of Ni metal and formation of coking, while intermediate carbonous species of *CH x (x = 0–3) can be gasified via the Sm 2 O 3 -Sm 2 O 2 CO 3 cycle. These Sm-promoted Ni-based catalysts are also tested with different temperatures and O/C, and show potentials in ATR of HAc for hydrogen production.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 8
·3594-3602
·
IF 2.7
Aihaimaitijiang Ababaikeri,Xueting Pan,Gulimeikereyi Tuniyazi,Xiangzhan Jiang,Yanhui Zhang,Dilnur Malik
A new non-centrosymmetric silicate Ba5Y12Zn[O(SiO4)]8 (BYZSO), the first compound of the Ba–Y–Zn–Si–O system, was synthesized by a high-temperature solution method in an open system, and its structure was identified using single-crystal X-ray diffraction data. Structural analysis indicates that it crystallizes in the noncentrosymmetric space group I2m (no. 121) with lattice parameters a = 18.7014(6) Å and c = 5.3640(2) Å corresponding to a tetragonal crystal system and is composed of isolated [ZnSi4O16] and [SiO4] units. Meanwhile, the effect of the cation-to-silicon ratio on the Si–O framework was also studied by investigating the structures of barium-, yttrium-, and zinc-containing silicates found in the Inorganic Crystal Structure Database (ICSD). Experimental characterization demonstrates that it possesses a short ultraviolet cut-off edge of 204 nm (6.18 eV), a moderate second harmonic generation (SHG) response (0.3× KDP) at the maximum particle size, and excellent thermal stability. Besides, first-principles theoretical calculations were carried out to elucidate the relationship between the electronic structure and optical properties. In summary, this work is instructive for the synthesis and design of silicates with different dimensions in the Ba–Y–Zn–Si–O system.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 7
·1-13
·
IF 5.3
Li Ziqiang,Liang Shuang,Zhang Changsheng,Zhou Li,Luo Fengjian,Lou Zhengyun,Chen Zongmao,Zhang Xinzhong,Yang Mei
A ratiometric fluorescence sensing strategy has been developed for the determination of Cu 2+ and glyphosate with high sensitivity and specificity based on OPD (o-phenylenediamine) and glutathione-stabilized gold nanoclusters (GSH-AuNCs). Water-soluble 1.75-nm size GSH-AuNCs with strong red fluorescence and maximum emission wavelength at 682 nm were synthesized using GSH as the template. OPD was oxidized by Cu 2+ , which produced the bright yellow fluorescence oxidation product 2,3-diaminophenazine (DAP) with a maximum fluorescence emission peak at 570 nm. When glyphosate existed in the system, the chelation between glyphosate and Cu 2+ hindered the formation of DAP and reduced the fluorescence intensity of the system at the wavelength of 570 nm. Meanwhile, the fluorescence intensity at the wavelength of 682 nm remained basically stable. It exhibited a good linear relationship towards Cu 2+ and glyphosate in water in the range 1.0–10 µM and 0.050–3.0 µg/mL with a detection limit of 0.547 µM and 0.0028 µg/mL, respectively. The method was also used for the semi-quantitative determination of Cu 2+ and glyphosate in water by fluorescence color changes visually detected by the naked eyes in the range 1.0–10 µM and 0.30–3.0 µg/mL, respectively. The sensing strategy showed higher sensitivity, more obvious color changes, and better disturbance performance, satisfying with the detection demands of Cu 2+ and glyphosate in environmental water samples. The study provides a reliable detection strategy in the environment safety fields. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Qiang-Qiang Yang,Zhi-Han Ma,Qiang Zhang,Zi-Han Song,Hong-Xiang Nie,Jing-Jing Pang,Zhao-Quan Yao,Hongliang Huang,Min Feng,Tong-Liang Hu,Jian Xu
One-step adsorptive separation of high-purity ethylene (C 2 H 4 ) from the mixtures with ethane (C 2 H 6 ) or propylene (C 3 H 6 ) is of crucial importance in the petrochemical industry. Nevertheless, the development of porous materials that possess both high adsorption capacities and selectivities of C 2 H 6 and C 3 H 6 over C 2 H 4 is still a formidable challenge. Herein, we present a microporous pillar-layered metal–organic framework (MOF) that exhibits excellent uptake capacities of C 2 H 6 (4.73 mmol g −1 ) and C 3 H 6 (8.05 mmol g −1 ) at 298 K and 1 bar, leading to high adsorption selectivities for equimolar mixtures of C 2 H 6 /C 2 H 4 (1.6) and C 3 H 6 /C 2 H 4 (16.4), respectively. Breakthrough column experiments demonstrate that the MOF could achieve one-step acquisition of polymer-grade C 2 H 4 (> 99.9 %) during C 2 H 6 /C 2 H 4 and C 3 H 6 /C 2 H 4 separations. Noteworthily, for a C 3 H 6 /C 2 H 4 mixture (2/5, v / v ), high-purity C 2 H 4 (> 99.9 %) and C 3 H 6 (> 99.5 %) can be directly harvested or recovered upon desorption, with high productivities of 86.23 and 31.05 L kg −1 , respectively, surpassing many well-developed adsorbents for C 3 H 6 /C 2 H 4 separation. Theoretical calculations reveal that the nonpolar pore surface bearing accessible N and O atoms affords more hydrogen bonding interactions with C 2 H 6 and C 3 H 6 than C 2 H 4 , accounting for the adsorption affinity in the order of C 3 H 6 > C 2 H 6 > C 2 H 4 . This work may offer valuable insights into the design and construction of high-performance MOFs for one-step C 2 H 4 purification.
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FOOD RESEARCH INTERNATIONAL
·
2024
·
IF 7
Shiya Gan,Yingqi Chen,Lei Zhao,Xiaoyi Zhao,Tong Qiu,Xiaoting Zhai,Qianying Dai
Chinese Xiaokeng green tea (XKGT) possesses elegant and fascinating aroma characteristics, but its key odorants are still unknown. In this study, 124 volatile compounds in the XKGT infusion were identified by headspace-solid phase microextraction (HS-SPME), stir bar sorptive extraction (SBSE), and solvent extraction-solid phase extraction (SE-SPE) combined with gas chromatography-mass spectrometry (GC–MS). Comparing these three pretreatments, we found HS-SPME was more efficient for headspace compounds while SE-SPE was more efficient for volatiles with higher boiling points. Furthermore, SBSE showed more sensitive to capture ketones then was effective to the application of pretreatment of aroma analysis in green tea. The aroma intensities (AIs) were further identified by gas chromatography–olfactometry (GC-O). According to the AI and relative odor activity value (rOAV), 27 compounds were identified as aroma-active compounds. Quantitative descriptive analysis (QDA) showed that the characteristic aroma attributes of XKGT were chestnut-like, corn-like, fresh, and so on. The results of network analysis showed that ( E , Z )-2,6-nonadienal, nonanal, octanal and nerolidol were responsible for the fresh aroma. Similarly, dimethyl sulfide, ( E , E )-2,4-heptadienal, ( E )-2-octenal and β -cyclocitral contributed to the corn-like aroma. Furthermore, indole was responsible for the chestnut-like and soybean-like aroma. This study contributes to a better understanding of the molecular mechanism of the aroma characteristics of XKGT.
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FUEL
·
2025
·
IF 7.5
Yake Wu,Suning Li,Jiawen Zhang,Shuai Li,Tao Zhong,Yanlong Zhu,Hong Li,Liuting Zhang
By constructing Ni-O-Zr interfaces, oxygen vacancies were generated and the interaction between the metal and the support in the catalyst was significantly enhanced. This synergy between Ni 0 and oxygen vacancies greatly boosted the catalytic activity of Ni 50 /ZrO 2 in the hydrogen storage system. Experimental tests showed that the MgH 2 + 10 wt%Ni 50 /ZrO 2 composite had a reduced initial hydrogen desorption temperature of 194.5 °C and released 6.30 wt%H 2 within 10 min at 265 °C. Notably, this composite exhibited excellent low-temperature hydrogen absorption kinetics, initiating absorption at 29 °C and nearly completing it (6.67 wt%H 2 ) at 134 °C. Furthermore, the activation energy for the modified MgH 2 had been substantially decreased from 76.66 kJ/mol to 32.01 kJ/mol (absorption) and 155.84 kJ/mol to 83.93 kJ/mol (desorption), respectively. The presence of oxygen vacancies at the Ni-O-Zr interface significantly amplified the catalyst’s charge conduction capabilities and provided a promising avenue for the development of effective catalysis for robust hydrogen storage.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Jie Zhou,Xianxin Qiu,Kaiqi Su,Gaixia Xu,Ping Wang
Based on the inhibition of okadaic acid (OA) on protein phosphatase 2A (PP2A), we developed disposable poly- o -aminophenol-carbon nanotubes (PoAP-CNTs) modified screen print electrode (SPE)-based electrochemical enzyme sensor for OA detection. Electropolymerized PoAP-CNTs composite film was coated on electrode for the immobilization of PP2A. Owing to the excellent physicochemical characteristic of PoAP-CNTs film, the performance of enzyme sensor was enhanced. Under the optimal conditions, the biosensor provides a larger linear range, and lower detection limit for the analysis of OA compared with colorimetric PP2A inhibition assay and PP2A/SPE. The spiked OA shellfish samples were applied to verify the efficiency of method for OA detection. The results shows acceptable recovery rate and low RSD, demonstrating the applicability of this method for in suit OA assessment in the quality and toxicity monitoring of seafood.
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SYNTHETIC METALS
·
2014
·
IF 2.222
Fang Liao,Siwei Yang,Xiubing Li,Lijun Yang,Zhihui Xie,Chenshu Hu,Ling He,Xinyuan Kang,Xun Song,Tongyan Ren
Poly(o-phenylenediamine) and benzeneselenol copolymer fluorescent nanorods were synthesized via a simple hydrothermal treatment and a novel, simple and ultra-sensitive oxidation–reduction fluorescent switch system was prepared based on these copolymer fluorescent nanorods. This switch system can be triggered by redox procedure. When this copolymer is oxidized by H 2 O 2 , the switch is “off”. The switch system is “on” when glutathione (GSH) is added. This switch system has good stability, excellent selectivity and specificity. What is more, the low detective limit indicates (detection limit: 10 −12 M) this switch system can be used as an ultra-sensitive fluorescent probe for H 2 O 2 or GSH. For the mechanism of switch processes, XPS results show the change of binding mode of Se in this copolymer is the main cause.
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CHINESE JOURNAL OF CATALYSIS
·
2013
·
IF 1.304
Qi SONG,Jiaying CAI,Junjie ZHANG,Weiqiang YU,Feng WANG,Jie XU
Phenethyl phenyl ether (PPE) was selected as a typical lignin model compound and hydrogenated and cleaved over two readily accessible nickel-based catalysts, which could be easily separated from the product mixture. The results revealed that the reduction of the nickel catalyst with gaseous hydrogen produced a species capable of achieving higher activity towards C-O-C bond cleavage compared to the Ru/C and Pd/C catalysts. The selectivity of the C-O-C bond cleavage over the Ni/C catalyst was 85%, and higher than the corresponding values in the Ru/C (40%) and Pd/C (69%) systems. Using the carbothermal reduction method for the production of the Ni/C-C catalyst, the conversion and selectivity levels reached 99%, with 40% of the benzene rings in PPE being reserved. In comparison, no benzene ring containing products wer observed over the noble metal catalysts. This difference was attributed to the interaction between the carbon support and the nickel nanoparticles. 摘要 研究了Ni基催化剂上木质素模型化合物苯基苯乙醚中C–O–C键加氢裂解性能. 结果表明, 14;Ni/C催化剂显示出优异的加氢裂解能力, 14;苯基苯乙醚的转化率达到99%以上. Ni/C催化剂的还原方法对裂解选择性有重要影响; 氢气还原制备的Ni/C-H催化剂上, 14;C–O–C键裂解选择性为85%. Ru/C和Pd/C催化剂上裂解选择性分别为40%和69%. 采用碳热还原方法制备的Ni/C-C催化剂, 14;可以实现高选择性加氢和裂解, 14;C–O–C键裂解选择性达到99%以上, 14;其中芳烃化合物收率为44%. 这可能与镍组分和载体碳之间的相互作用有关.
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CATALYSIS LETTERS
·
2015
·Vol. 145
·期 3
·784-793
·
IF 2.307
Zhang Xuejun,Zhang Peipei,Yu Hongbo,Ma Zhen,Zhou Shenghu
Abstract Bimetallic PdM (M = Ni, Co, Fe) nanoparticles were synthesized using butyllithium as a reductant, and were used to prepare Pd–M
x
O
y
/KIT-6 catalysts by appropriate oxidation and reduction treatments. These catalysts showed higher selectivity in the hydrogenation of p -chloronitrobenzene to p -chloroaniline than Pd/KIT-6. Relevant characterization was conducted using X-ray diffraction, transmission electron microscopy, N 2 adsorption–desorption, X-ray photoelectron spectroscopy, inductive coupled plasma emission spectrometer, and H 2 temperature-programmed reduction. Graphical Abstract
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Jingyan Zhou,Fei Wu,Zhexin Zhu,Tiefeng Xu,Wangyang Lu
Phthalocyanine has been used widely as an oxidation catalyst, e.g., in wastewater treatment. It has become important and necessary to study phthalocyanine derivatives, to understand the potential effect they may have. Despite the fact that phthalocyanine dimers are easy to generate, such complexes have been ignored as catalysts. We prepared O-bridged iron perfluorophthalocyanine dimers (FePcF 16 -O-FePcF 16 ). Ultraviolet–visible, X-ray diffractometry, X-ray photoelectron spectroscopy, density-functional theory analysis and electrospray ionization–mass spectrometry technology assisted by pyridine ligands have been used to identify the structure of FePcF 16 -O-FePcF 16. Carbamazepine selected as a model pollutant could be effectively oxidized in the system with FePcF 16 -O-FePcF 16 and H 2 O 2 . Electron paramagnetic resonance data indicated an active center that was different from OH in the Fenton reaction. Electrospray ionization–mass spectrometry detected the generation of high-valent diiron-oxo species, which implies that carbamazepine degradation was accomplished by the attack of Fe IV O Fe IV O in the FePcF 16 -O-FePcF 16 /H 2 O 2 system. Thus, we identified an O-bridge iron perfluorophthalocyanine dimer and proposed a catalytic mechanism. These results may provide a novel explanation for the oxidative mechanism.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yibing Xie,Xueqian Wang,Zan Qu,Ping Ning,Langlang Wang,Haomiao Xu,Wenjun Huang,Jichang Lu,Jianfei Luo
The transformation of toxic arsine (AsH3) gas into valuable elemental arsenic (As0) from industrial exhaust gases is important for achieving sustainable development goals. Although advanced arsenic removal catalysts can improve the removal efficiency of AsH3, toxic arsenic oxides generated during this process have not received adequate attention. In light of this, a novel approach for obtaining stable As0 products was proposed by performing controlled moderate oxidation. We designed a tailored Ni-based catalyst through an acid etching approach to alter interactions between Ni and NaY. As a result, the 1Ni/NaY-H catalyst yielded an unprecedented proportion of As0 as the major product (65%), which is superior to those of other reported catalysts that only produced arsenic oxides. Density functional theory calculations clarified that Ni species changed the electronic structure of oxygen atoms, and the formed [NiIII–OH (μ-O)] active centers facilitated the adsorption of AsH2*, AsH*, and As* reaction intermediates for As–H bond cleavage, thereby decreasing the direct reactivity of oxygen with the arsenic intermediates. This work presents pioneering insights into inhibiting excessive oxidation during AsH3 removal, demonstrating potential environmental applications for recovery of As0 from toxic AsH3.
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