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FUEL PROCESSING TECHNOLOGY · 2019 · IF 4.507

Metal-organic framework containing Brønsted acidity and Lewis acidity for efficient conversion glucose to levulinic acid

Haonan Qu,Bingyi Liu,Guohua Gao,Yiming Ma,Yanmei Zhou,Hua Zhou,Li Li,Yonghong Li,Shengjian Liu

Levulinic acid (LA) is a versatile key building block in the conversion of carbohydrates and it is an important basic chemical with various potential uses. MIL-100(Fe) loading with insoluble lysine functionalized phosphotungstic acid (Lys-PM 2 ) as heterogeneous catalysts have been synthesized for the conversion of glucose to LA in water. The optimized yield of LA is obtained by using Lys-PM 2 to catalyze glucose conversion is comparable to the majority of effective catalysts. The highest yield of LA (57.9%) is obtained at 150 °C for 9 h with 100 mg glucose and 25 mg Lys-PM 2 , since the Brønsted acidity and Lewis acidity of Lys-PM 2 . And the catalyst is able to recycle at least four times. It demonstrates the potential of Lys-PM 2 for the conversion of biomass.

研究领域: 催化化学 · 绿色化学 · 生物质能源 · 有机转化 · 材料化学 · 可持续化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF SOILS AND SEDIMENTS · 2016 ·Vol. 17 ·期 2 ·536-542 · IF 2.206

The effect of different TiO2 nanoparticles on the release and transformation of mercury in sediment

Zhang Jinyang,Li Chuxian,Wang Dingyong,Zhang Cheng,Liang Li,Zhou Xiong

Purpose The environmental safety of both nano-TiO 2 particles and mercury (Hg) pollution has been of widespread concern. Soils and sediments were the main receiving environments of nano-TiO 2 and Hg. There was a strong association between nano-TiO 2 with Hg compounds. Very limited research has been carried out on the impact of nano-TiO 2 on the environmental behavior of Hg in sediments. The objective of this study was to investigate the effects of nano-TiO 2 on the release and transformation of Hg in sediments. Materials and methods Two types of TiO 2 nanoparticles were employed. Sediment samples were collected in the water level fluctuating zone of the Three Gorges Reservoir, China. Sediment samples spiked with HgCl 2 solution were taken as Hg-contaminated sediments. The flooding experiments were conducted using capped borosilicate glass bottles containing 300 ml TiO 2 suspensions (0.2 g L −1 and 0.4 g L −1 ) and 30 g original or Hg-contaminated sediment samples outdoors. All experiments were conducted in triplicate. Water samples were collected at determined interval times over a 60-day period. Sediments were collected on the 60th day. Total Hg (THg) and methylmercury (MHg) in both water and sediment samples and Hg speciation just in sediment samples were determined. A series of control samples without TiO 2 addition were also prepared. Results and discussion The results showed that nano-TiO 2 particles at high content (4 g kg −1 ) promoted the release of Hg in sediments, and the anatase particles showed a stronger effect. Methyl Hg concentrations in waters of nano-TiO 2 treatments significantly decreased by the 10th day. The effect of nano-TiO 2 greatly depended on anatase and rutile particles. After that, methyl Hg concentrations had no significant difference between nano-TiO 2 treatments and the control, except 2 g kg −1 rutile treatment by the 20th day. The changes of Hg speciation in sediments demonstrated that nano-TiO 2 inhibited the transformation of Hg-bound organic matter into the oxidated state, especially upon 2 g kg −1 rutile treatment. This was consistent with the lower MHg concentrations in the 2 g kg −1 rutile treatment. Conclusions Both anatase and rutile nano-TiO 2 were found to affect the release of Hg in sediment. Nano-TiO 2 promoted THg release in sediments and posed an increased risk of Hg contamination in waters, especially for anatase particles. Moreover, nano-TiO 2 inhibited the methylation process of Hg in sediments at the initial stage of flooding and could affect the transformation of Hg speciation in sediments, especially for low-content rutile particles.

研究领域: 环境科学 · 地球化学 · 水体生态学 · 污染控制 · 环境毒理学
✓ 已验证 DOI 高影响因子
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WATER AIR AND SOIL POLLUTION · 2019 ·Vol. 230 ·期 2 ·41 · IF 1.774

Formation of Multiple Nitrosamines from the Ozonation of Corresponding Precursor Secondary Amines: Influencing Factors and Transformation Mechanisms

Wang Wanfeng,Liang Fang,Guo Yanling,Wu Ruijie,Pan Feng,Jin Caixia,Wang Jun

Since nitrosamine disinfection by products is highly carcinogenic, they have attracted considerable attention due to their increased presence in ambient waterways and potable water supplies. For the present study, the potential formation of nitrosamines from corresponding precursor secondary amines during ozonation was investigated. The results revealed that five nitrosamines were observed during the ozonation of their corresponding secondary amines. The molar yields initially increased and then decreased with longer contact times and higher ozone doses. These phenomena indicated that ozone not only promoted nitrosamine formation but also degraded the formed nitrosamines. High pH had a positive influence on nitrosamine formation at room temperature. Further, coexisting substances including nitrate, nitrite, humic acid, and tert-butanol inhibited the generation of nitrosamines due to hydroxyl radical (·OH) competition and scavengers, whereas in the presence of hydroxylamine, nitrosamine formation increased considerably without ozone due to its capacity for independent formation between secondary amines and hydroxylamine. Further, the generation of nitrosamines from secondary amines was primarily attributed to O 3 and ·OH oxidation, which was produced through the decomposition of ozone. The transformation pathways were mainly comprised of the indirect routes between the O 3 /·OH intermediates. The findings of this study were helpful toward expanding the knowledge of nitrosamine formation during the corresponding precursor secondary amine ozonation process.

研究领域: 环境科学 · 水处理化学 · 污染物转化 · 消毒副产物 · 氧化过程
✓ 已验证 DOI 高影响因子
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Small · 2022 ·Vol. 18 ·期 48 ·2205163 · IF 15.153

Self-Supporting Multicomponent Hierarchical Network Aerogel as Sulfur Anchoring-Catalytic Medium for Highly Stable Lithium–Sulfur Battery

Shuhao Tian,Juanjuan Huang,Hongcen Yang,Guo Liu,Qi Zeng,Di Wang,Xiao Sun,Kun Tao,Guohan Liu,Shanglong Peng

The low utilization rate of active materials, shuttle effect of lithium polysulfides (LiPSs), and slow reaction kinetics lead to the extremely low efficiency and poor high current cycle stability of lithium sulfur batteries (Li–S batteries). In this paper, a self-supporting multicomponent hierarchical network aerogel is proposed as the modified cathode (S/GO@MX@VS 4 ). It consists of graphene (GO) and MXene nanosheets (MX) loaded with VS 4 nanoparticles. The experimental results and first-principles calculations show that the GO@MX@VS 4 aerogel has strong adsorption and reversible conversion effects on LiPSs. It can not only inhibit the shuttle effect and improve the utilization rate of active substances by keeping the chain crystal structure of VS 4 , but also promote the reversibility and kinetics of the reaction by accelerating the liquid–solid transformation in the reduction process and the decomposition of insoluble Li 2 S in the oxidation process. The GO@MX@VS 4 aerogel modified cathode with a multicomponent synergy exhibits the capacity ratios (Q 1 /Q 2 ) at different discharge stages is close to the theoretical value (1:2.8), and the capacity decay per cycle is 0.019% in 1200 cycles at 5C. Also, a high areal capacity of 6.90 mAh cm −2 is provided even at high sulfur loading (7.39 mg cm −2 ) and low electrolyte/sulfur ratio (E/S, 8.0 µL mg −1 ).

研究领域: 电化学储能 · 材料科学 · 纳米材料 · 能源化学 · 电池技术 · 表面催化
✓ 已验证 DOI 高影响因子
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CATALYSIS COMMUNICATIONS · 2011 ·Vol. 15 ·期 1 ·52-55 · IF 2.827

Selective epoxidation of alkenes with hydrogen peroxide over efficient and recyclable manganese oxides

Ben Qi,Lan-Lan Lou,Kai Yu,Wenyue Bian,Shuangxi Liu

A series of manganese oxides (MnO, Mn 3 O 4 , Mn 2 O 3 and MnO 2 ) were prepared and firstly applied as heterogeneous catalysts for the liquid phase epoxidation of alkenes with 30% H 2 O 2 in bicarbonate solution. Under our experimental conditions, MnO exhibited superior activity for the conversion of styrene to achieve ca. 100% with 92.4% selectivity of epoxide, compared to the other three manganese oxides as well as other metal oxides. Furthermore, recycling studies showed the good recyclability of MnO as a heterogeneous catalyst, which did not lose the catalytic activity after four reuses appreciably.

研究领域: 催化化学 · 有机合成 · 材料化学 · 绿色化学 · 工业化学
✓ 已验证 DOI 高影响因子
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Reaction Chemistry & Engineering · 2023 ·Vol. 8 ·期 10 ·2632-2640 · IF 3.9

Low-temperature conversion of CaO-captured CO2 to CH4 over a greenly prepared Ni/CaO/Al2O3 composite under static pressure conditions

Han-Qing Chen,Zhan-Kuo Guo,Shu-Xiang Xiang,Hui-Lin Jiang,Yun-Lei Teng

Directly converting metal oxide-adsorbed CO2 to CH4 at low temperatures is a more energy-saving method for achieving carbon capture and utilization. In this study, an Al2O3-supported Ni/CaO composite was greenly prepared by a mechanochemical method. It is found that CO2 capture and selective methanation can be realized over the Ni/CaO/Al2O3 composite at as low as 200 °C under static pressure conditions. The methane yields over the 10Ni/10CaO/γ-Al2O3 composite reach 70.05 and 388.5 μmol CH4 per g at 200 and 350 °C with approximately 100% selectivity to CH4. The experimental results show that the reaction time and temperature obviously affect the methanation yield over the Ni/CaO/Al2O3 composite. This work provides a facile energy-saving strategy for converting CO2 to CH4 at low temperatures.

研究领域: 环境催化 · 能源化学 · 材料科学 · 工业化学 · 碳捕集与利用
✓ 已验证 DOI 高影响因子
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MACROMOLECULAR MATERIALS AND ENGINEERING · 2018 ·Vol. 304 ·期 1 ·1800477 · IF 2.69

Chemically Modified Polyvinyl Butyral Polymer Membrane as a Gel Electrolyte for Lithium Ion Battery Applications

Ziqiang Xu,Wenlei Li,Zhi Chen,Dongxia Wang,Tingting Feng,Hanna Potapenko,Mengqiang Wu

A novel porous membrane of chemically modified polyvinyl butyral (mPVB), with improved thermal properties and chemical stability for lithium ion battery applications, is successfully synthesized by utilizing the chain extension reaction of the OH units from PVB. The porous mPVB membranes are obtained via the tape casting and phase inversion method. The corresponding gel polymer electrolyte (GPE) is achieved by immersing the as-prepared membranes in the liquid electrolyte. The electrochemical performances of the GPE show that the mPVB membranes have the features of good uniformity, high porosity ( ≈ 90%), great thermal stability, and high mechanical strength. Moreover, the GPE exhibits good chemical stability, a wide electrochemical window, as well as high ionic conductivity ( ≈ 1.21 × 10 −3 S cm −1 ). A test of a Li/GPE/LiFePO 4 battery cell shows a capacity of 147.7 mAh g −1 and excellent cycling stability, demonstrating the great potential of the mPVB-based GPE for lithium ion battery applications.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 电池技术
✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Spatially controlled oxygen storage materials improved the syngas selectivity on chemical looping methane conversion

Dewang Zeng,Yu Qiu,Min Li,Li Ma,Dongxu Cui,Shuai Zhang,Rui Xiao

Chemical looping redox cycle of oxygen storage materials offers a versatile platform to convert methane to value-added products in a clean and efficient manner. However, the highly dynamic nature of the oxygen diffusion process restrains the selective formation of the target products over a long reaction period. In this work, we show the oxygen storage materials-comprising of iron oxides and zirconium oxide support, with the nickel catalyst controllably deposited—that significantly enhanced the syngas selectivity. Mechanistic study indicated the oxygen releasing rate can be well controlled within a long reaction period by the specific spatial structure, demonstrating a new strategy to tune the oxygen diffusion in chemical looping process. Through the observed spatial effects, this work can be also extended to develop more oxygen storage materials for the other chemical looping applications, e.g. methane reforming, methane oxidative coupling, ethane oxidative dehydrogenation, etc .

研究领域: 催化化学 · 能源化学 · 材料化学 · 化学工程 · 多相催化
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Accelerated adsorption of tetracyclines and microbes with FeOn(OH)m modified oyster shell: Its application on biotransformation of oxytetracycline in anaerobic enrichment culture

Shujuan Lian,Xiaoshuang Shi,Mingyi Lu,Mengdan Zhang,Xiaohuan Dong,Xu Li,Quan Feng,Rongbo Guo

Due to the persistence in residue and the emission to environment, antibiotics have become the emerging contaminants. Tetracyclines, as the largest amount of antibiotics in the breeding industry, were investigated in this study. For eliminating the tetracyclines, anaerobic culture was enriched from livestock waste after four generations and FeOn(OH)m modified oyster shell powders (OSPs) were amended into the enrichment culture as auxiliary method. Tetracycline and oxytetracycline were selected as the model compounds. The adsorption models (Langmuir and Freundlich isotherms) of tetracycline and microbes on OSPs were simulated respectively. With the addition of FeOn(OH)m modified OSPs, the transformation efficiency of oxytetracycline achieved 81.5% after 22 days’ incubation, approximately 1.85 times higher than the 4th generation (G-IV) enrichment culture without modified OSPs. Dehydration, demethylation, dehydroxylation and decarboxylation took place under anaerobic condition, inferred from the detected metabolites transformed from oxytetracycline. Genus Methanosarcina and two operational taxonomic units (OTUs) assigned to order Clostridiales , showed an increasing trend on abundance, indicating the contribution to transformation of oxytetracycline. Therefore, the FeOn(OH)m modified OSPs and enrichment culture can accelerate the transformation of oxytetracycline simultaneously, indicating a promising utilization not only for waste water system but also for antibiotic contaminated biomass treatment.

研究领域: 环境微生物学 · 污染物生物降解 · 环境工程 · 抗生素去除 · 吸附材料 · 厌氧消化 · 药物代谢
✓ 已验证 DOI 高影响因子
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Journal of Environmental Sciences · 2024 · IF 5.9

Coupled transformations of manganese and dissolved organic matter molecules during iron (oxyhydr)oxide-catalyzed oxidation of Mn(II)

Xixian Huang,Bing Yang,Ye Dou,Yang Ding

The abiotic oxidation of divalent manganese (Mn(II)) and the formation of Mn oxides are important geochemical processes, which control the mobility and availability of Mn as well as element cycling and pollutant behavior in soils. It was found that iron (oxyhydr)oxides can catalyze Mn(II) oxidation , but the effects of the coexisting dissolved organic matter (DOM) molecules on the catalysis of different iron (oxyhydr)oxides for Mn(II) oxidation are poorly understood. Herein, we investigated Mn(II) oxidation under the impacts of the interactions between iron (oxyhydr)oxides (i.e., ferrihydrite, goethite and hematite) and DOM molecules. Simultaneously, we elucidated the variations of DOM composition and properties. Our results indicated that the catalysis of iron (oxyhydr)oxides for Mn(II) oxidation was significantly inhibited by DOM. Moreover, DOM had less inhibiting effect on the catalysis of ferrihydrite for Mn(II) oxidation and the formation of Mn oxides (e.g., hausmannite and buserite) relative to goethite and hematite, which was partially because of the higher electron transfer capacities of ferrihydrite. Meanwhile, DOM molecules with high nominal oxidation state of carbon (NOSC), molecular weight, unsaturation and aromaticity were selectively adsorbed and oxidized by Mn oxides , including the oxygenated phenols and polyphenols. The newly formed molecules mainly belonged to phenols depleted of oxygen and aliphatics. Furthermore, NOSC was a key molecular characteristic for controlling DOM composition during DOM adsorption and oxidation by Mn oxides when iron minerals were present. Overall, our research contributes to understanding Mn(II) oxidation mechanisms under heterogeneous systems and behaviors of DOM molecules in the environment.

研究领域: 环境地球化学 · 土壤化学 · 水文地球化学 · 有机-矿物相互作用 · 元素生物地球化学循环
✓ 已验证 DOI 高影响因子
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Journal of Environmental Chemical Engineering · 2022 ·Vol. 10 ·期 6 ·108837 · IF 7.968

Engineering oxygen vacancy and crystal surfaces for TiO2-based photocatalysts for enhanced photocatalytic hydrogenation of bio-based carbonyls to biofuels

Yumei Jian,Ye Meng,Jie Li,Hongguo Wu,Shunmugavel Saravanamurugan,Hu Li

Photocatalytic reductive conversion of bio-derivatives to biofuels and fine chemicals is an eco-friendly and energy-saving way for biomass valorization. Herein, we developed a new and high-performance protocol for control of activity/selectivity in photocatalytic reductive upgrading of biomass to biofuels at room temperature via engineering oxygen vacancy (Ov) and manipulating the exposed crystal surfaces of the TiO 2 -based catalysts, such as efficient cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to γ-valerolactone in water (up to 96% yield, TOF: 112.1 h −1 ), and the selective conversion of 5-methylfurfural to 5-methylfurfuryl alcohol (90% yield) or long carbon-chain coupling products (86% yield) in methanol, respectively. The {101} crystal plane is prone to produce more Ov in situ than the {001} and {110} crystal planes. The formation of Ov was not only beneficial to the adsorption and activation of the bio-based carbonyls, but also could enhance the migration efficiency of the photo-generated carriers and effectively adjust the semiconductor band structure of the TiO 2 -based photocatalyst to promote the visible-light absorption, thus enhancing the overall reductive conversion process, as elucidated by DFT calculations. Also, the charge distribution and adsorption intensity of different exposed crystal surfaces of the photocatalyst were able to control the selectivity of the bioproducts . In addition, the optimal Ov-TiO 2− x {101} catalyst had excellent reusability and could be reused at least five times with no obvious decrease in photocatalytic performance. The strategy of selectivity control via engineering the catalyst exposed crystal surfaces and loaded Ov provides an opportunity for multi-catalytic biomass conversion to biofuels.

研究领域: 催化化学 · 材料科学 · 能源化学 · 环境科学 · 绿色化学 · 表面科学 · 光催化
✓ 已验证 DOI 高影响因子
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Journal of Energy Chemistry · 2021 · IF 9.676

A novel carbon cycle process assisted by Ni/La2O3 catalyst for enhanced thermochemical CO2 splitting

Yu Kang,Yujia Han,Cong Wei,Kuo Liu,Ming Tian,Chuande Huang,Chaojie Wang,Jian Lin,Baolin Hou,Xiaoli Pan,Yang Su,Lin Li,Riguang Zhang,Yong Hao,Xiaodong Wang

Thermochemical two-step CO 2 splitting is a potential approach that fixes the sustainable resource into transportable liquid fuels. However, the harsh CO 2 splitting conditions, the limited oxygen release kinetics and capacity of metal oxides block further promoted the CO yield and solar-to-fuel energy efficiency. Here, we propose a different carbon cycle assisted by Ni/La 2 O 3 via coupling methane decomposition with thermochemical CO 2 splitting, replacing conventional metal oxides cycle. Superior performance was demonstrated with methane conversion reached around 94% with almost pure H 2 generation. Encouragingly, CO 2 conversion of 98% and CO yield of 6.9 mmol g −1 derived from CO 2 were achieved, with peak CO evolution rate (402 mL min −1  g −1 ) of orders of magnitude higher than that in metal oxide process and outstanding thermodynamic solar-to-fuel energy efficiency (55.5% vs. 18.5%). This was relevant to the synergistic activation of La 2 O 3 and Ni for CO 2 in carbon cycle, thus improving CO 2 splitting reaction with carbon species.

研究领域: 能源化学 · 催化化学 · 可持续能源 · 热化学转化 · 二氧化碳利用
✓ 已验证 DOI 高影响因子
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