Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 12
·6375-6383
·
IF 11.9
Yixuan Feng,Kun Yang,Richard L. Smith,Xinhua Qi
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) is an efficient and sustainable way to produce a 2,5-furandicarboxylic acid (FDCA) monomer. In this study, two-dimensional (2D) metal–organic framework (MOF) nanoarrays embedded with Ni/Co/Fe sulfide nanoclusters were employed as electrocatalysts for HMF oxidation. The as-prepared NiCoFeS-MOF catalyst had interlaced structures and achieved 100% HMF conversion, 99% FDCA yields and Faraday efficiencies as high as 99% at 1.39 V vs. RHE driving voltage. Combination of metal sulfide nanoclusters with 2D MOF nanoarrays greatly enlarged the electrochemical active surface area and increased the number of active catalytic sites while improving electron transport. X-ray photoelectron spectroscopy indicated that electronic interactions increased the electron density of metal sites and enhanced intrinsic NiCoFeS-MOF electrooxidation performance. Embedding metal sulfide nanoclusters into MOF nanoarrays using the simple one-step solvothermal method proposed in this work greatly expands the scope of electrode materials available for electrochemical upgrading of biomass-related compounds.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 7
·3040
·
IF 4.6
Lei Zhao,Shichao Du,Rui Gong,Wanqi Jia,Zhimin Chen,Zhiyu Ren
The renewable-energy-driven integration of hydrogen production and biomass conversion into value-added products is desirable for the current global energy transition, but still a challenge. Herein, carbon-coated CoO–Co heterojunction arrays were built on copper foam (CoO–Co@C/CF) by the carbothermal reduction to catalyze the hydrogen evolution reaction (HER) coupled with a 5-hydroxymethylfurfural electrooxidation reaction (HMFEOR). The electronic modulation induced by the CoO–Co heterojunction endows CoO–Co@C/CF with a powerful catalytic ability. CoO–Co@C/CF is energetic for HER, yielding an overpotential of 69 mV at 10 mA·cm−1and Tafel slope of 58 mV·dec−1. Meanwhile, CoO–Co@C/CF delivers an excellent electrochemical activity for the selective conversion from HMF into 2,5-furandicarboxylic acid (FDCA), achieving a conversion of 100%, FDCA yield of 99.4% and faradaic efficiency of 99.4% at the lower oxidation potential, along with an excellent cycling stability. The integrated CoO–Co@C/CF||CoO–Co@C/CF configuration actualizes the H2O–HMF-coupled electrolysis at a satisfactory cell voltage of 1.448 V at 10 mA·cm−2. This work highlights the feasibility of engineering double active sites for the coupled electrolytic system.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hao Zhang,Runze Zhang,Wendi Zhang,Bang Gu,Qinghu Tang,Qiue Cao,Wenhao Fang
Constructing functionalized surface for heterogeneous catalysts is vital toward effective conversion of biomass. We show that Pt nanoparticles (ca. 2.1 nm) loaded on Co-Nb bimetallic oxide can efficiently catalyze the aqueous-phase base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid. We ingeniously construct different surface element-distributions over three Co-Nb oxides (Nb@Co, Co&Nb and Co@Nb) with the same bulk composition by changing precipitation sequence of Co and Nb precursors. This strategy allows rationally modulating synergistic interaction and surface acidity of Co-Nb oxides and in return boosts the pristine oxidation activity of loaded-Pt nanoparticles. We use kinetic investigations, comprehensive characterizations, and particularly in situ DRIFT-IR adsorption technique (CO, pyridine and furfural as probe molecules) to unravel the origin of synergistic catalysis. We disclose that Nb 5+ -enriched surface can formulate sufficient Lewis acidic sites and stabilize electron-rich Pt 0 active centers, accelerating the tandem oxidation of HMF and the intermediates. The Co@Nb-Pt catalyst shows the highest productivity of FDCA (25 mmol FDCA mol Pt –1 h –1 ) among all Pt catalysts in the literature and achieves > 99% yield of FDCA at 110 °C and 10 bar of O 2 .
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Guozhi Fan,Yi Chen,Yuchan Lu,Qunpeng Cheng,Bo Chai,Guangsen Song
UiO-66-derived H 2 N-UiO-66-SO 3 H with acid-base active sites was used for the co-production of 5-hydroxymethyl furfural (5-HMF) and furfural (FUR) in the direct conversion of holocellulose composed of cellulose and hemicellulose. The prepared catalyst was further characterized by various techniques, confirming its formation, structure, and composition. H 2 N-UiO-66-SO 3 H displayed excellent performance for the selective conversion of holocellulose to 5-HMF and FUR, achieving yields of 39.1 % and 28.2 %, respectively. The reusability of the catalyst was also investigated by direct use after recycling without any pretreatment. The results indicated that H 2 N-UiO-66-SO 3 H had good stability, and after four cycles, the yields of 5-HMF and FUR decreased only slightly to 37.2 % and 27.1 %, respectively. The recyclable catalyst H 2 N-UiO-66-SO 3 H for the effective conversion of holocellulose to 5-HMF and FUR demonstrated application potential for the utilization of lignocellulosic biomass.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 32
·78988-79000
·
IF 5.8
Dong Jiayu,Song Xianni,Zhang Shuchi,Tan Mengyu,Zhao Haiyan,Wu Donglei
A novel hierarchical Cu/ZSM-5 was prepared over alkaline treatment and incipient wet impregnation method for the catalytic ozonation of polyvinyl alcohol (PVA). Under the optimum preparation conditions, hierarchical Cu/ZSM-5 exhibited an excellent mineralization performance during the PVA degradation process, and the removal rate of TOC after 60 min of reaction was 47.86%, much higher than that of ozonation alone (5.40%). Its high catalytic activity could attribute to the large pore volume (0.27 cm 3 /g) and pore size (6.51 nm) which are beneficial for the distribution of loaded copper and adsorption performance for PVA. Compared to ·OH, 1 O 2 (2.66 times in 10 min) contributed more to the removal of PVA. The degradation of PVA was a combined process of direct ozone oxidation, catalytic ozonation and adsorption. With its high catalytic performance and stability, hierarchical Cu/ZSM-5 has a very broad application prospect in the process of catalytic ozonation of refractory pollutants.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GLYCOCONJUGATE JOURNAL
·
2023
·Vol. 40
·期 4
·435-448
·
IF 3
Bai Ruifeng,Wang Jingyi,Brockhausen Inka,Gao Yin
The presence of N -glycolylneuraminic acid (Neu5Gc), a non-human sialic acid in cancer patients, is currently attributed to the consumption of red meat. Excess dietary red meat has been considered a risk factor causing chronic inflammation and for the development of cancers. However, it remains unknown whether Neu5Gc can be generated via a chemical reaction rather than via a metabolic pathway in the presence of high levels of reactive oxygen species (ROS) found in the inflammatory and tumor environments. In this study, the conversion of N -acetylneuraminic acid (Neu5Ac) to Neu5Gc has been assessed in vitro under conditions mimicking the hydroxyl radical-rich humoral environment found in inflammatory and cancerous tissues. As a result, Neu5Gc has been detected via liquid chromatography-multiple reaction monitoring mass spectrometry. Furthermore, this conversion has also been found to take place in serum biomatrix containing ROS and in cancer cell cultures with induced ROS production.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF LUMINESCENCE
·
2023
·
IF 3.6
Fan Chen,Xiao-Jun Wang,Xuehu Zhang,Changhua Zhang
Lead-free halide perovskites have recently evoked considerable interest in illumination and display, due to their intriguing optical properties . Herein, we present an efficient and facile strategy to prepare Cs 2 InCl 5-x Br x ·H 2 O (x = 0–5) perovskites . The preparation was performed at a low temperature of 80 °C under atmospheric pressure, and required no complex technological process. Comparing with that prepared by the traditional hydrothermal method , the emission intensity of the prepared Cs 2 InX 5 ·H 2 O (X = Cl/Br) perovskites were increased by two times. Besides, Sb 3+ ions were successfully doped into the matrix of Cs 2 InX 5 ·H 2 O (X = Cl/Br) by our method. After doping with Sb 3+ , the emission intensities of Cs 2 InX 5 ·H 2 O were greatly enhanced, with enhanced by a factor of ∼187 and ∼102, respectively. Importantly, the PLQYs were greatly improved, reaching 79.6% and 42.7%, respectively. Additionally, the effects of Br − on luminescent properties of Cs 2 InCl 5-x Br x ·H 2 O:Sb 3+ (x = 0–5) were also investigated in this work. Though the control of the Br − content, tunable emissions from 575 nm to 630 nm were achieved. These results indicate the prepared samples could be promising environmentally-friendly materials for lightings. Furthermore, this work presents a reliable and simple method for preparing high-quality perovskites.
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 4
·1395-1405
·
IF 9.8
Pengfei Wu,Miao Yang,Jifeng Pang,Dong Fan,Lei Song,Tantan Sun,Mingyuan Zheng,Peng Tian,Tao Zhang
The conversion of biomass resources into 5-hydroxymethylfurfural (5-HMF) is of great significance for the valorization of biomass into key chemicals and fuels. However, designing heterogeneous catalysts with controllable Brønsted and Lewis acid sites for achieving high yields of 5-HMF remains a challenge. Herein, a highly efficient SAPO-34 nanocrystallites catalyst has been synthesized by a facile strategy, employing commercial low-cost organosilane [3-glycidoxypropyltrimethoxysilane (AC-230)] together with seeds and microporous template triethylamine. The complex functionalities of AC-230 were investigated by conditional experiments and systematic characterizations. The resultant SAPO-34 nanocrystallites (SP-MS) have an ultra-high external surface area (180 m2 g−1), large mesopore volume (0.51 cm3 g−1), a high amount of accessible Brønsted/Lewis acid, and good hydrophilicity. For the conversion of mono-, di-and poly-saccharides into 5-HMF, SP-MS exhibited remarkable activity. Typically, an 81% yield of 5-HMF with a complete glucose conversion was achieved in a biphasic NaCl–H2O/methyl isobutyl ketone solvent system at 170 °C within 45 min, obviously better than other heterogeneous acid catalysts. According to the kinetic study, the Lewis acid sites over SP-MS decreased the apparent activation energy (85 kJ mol−1) of glucose isomerization, and then the abundant Brønsted acid sites boosted the 5-HMF yields. More attractively, the catalytic activity can be restored after at least four cycles. This work is anticipated to provide insights into designing efficient and robust SAPO catalysts for 5-HMF production.
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Hao Zhang,Yinghao Wang,Qizhao Zhang,Bang Gu,Qinghu Tang,Qiue Cao,Kun Wei,Wenhao Fang
The base-free aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water is recognized as an important and sustainable upgrading process for cellulosic carbohydrates. However, selectivity control still remains a challenge. Here, we disclose that the unique synergy in magnetic Ni x Co 1 O y ( x = 1, 3 and 5) bimetallic oxides can induce reactive oxygen defects and simultaneously stabilize small-sized metallic Au nanoparticles in the Au/Ni x Co 1 O y catalysts. Such catalytic features render effective adsorption and activation of O 2 , OH and C O groups, realizing selective oxidation of HMF to FDCA . On a series of magnetic Au/Ni x Co 1 O y catalysts with almost identical Au loadings (ca. 0.5 wt%) and particle sizes (ca. 2.7 nm), the variable Ni/Co molar ratios give rise to the tunable electron density of Au sites and synergistic effect between NiO and CoO y . The initial conversion rates of HMF and its derived intermediates (i.e., DFF, HMFCA and FFCA) show a volcano-like dependence on the number of oxygen defects (i.e., O 2 − and O − ) and electron-rich Au 0 sites. The optimum Au/Ni 3 Co 1 O y catalyst exhibits a highest productivity of FDCA (12.5 mmol FDCA mol Au - 1 h −1 ) among all the Au catalysts in the literature and achieves > 99% yield of FDCA at 120 °C and 10 bar of O 2 . In addition, this catalyst can be easily recovered by a magnet and show superior stability and reusability during six consecutive cycling tests. This work may shed a light on Au catalysis for the base-free oxidation of biomass compounds by smartly using the synergy in bimetallic oxide carriers.
✓ 已验证
产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 3
·1-10
·
IF 5.7
Fan Xiaoyu,Zhang Shuai,Li Rui,Chen Yafei,Jiang Shuhan,Liu Tao,Shao Xiaodong,Wang Shuhao,Yue Qiaoli
Novel and portable cotton swab–based fluorometry was constructed for the first time for 3-aminosalicylic acid (3-ASA) and 5-aminosalicylic acid (5-ASA) detection. It was carried out by fluorescence enhancement on silver (Ag)–doped black phosphorus quantum dots (Ag@BPQD). Ag@BPQD were prepared from AgNO 3 and bulk black phosphorus in N, N-dimethylformamide (DMF) solution by solvothermal decomposition after mechanical exfoliation. Ag@BPQD show blue fluorescence with a quantum yield (QY) of 2.43%. In the presence of Ag@BPQD, 3-ASA exhibited bright blue fluorescence (λ ex = 328 nm, λ em = 448 nm). The fluorescence of 5-ASA was also enhanced significantly and exhibited bright green emission (λ ex = 328 nm, λ em = 484 nm). The linear range of 3-ASA is 0–90 μM with a detection limit (LOD) of 0.10 μM, relative standard deviation (RSD) ≤ 2.04%, and a recovery range of 98.0–104.3%. The linear range of 5-ASA is 0–120 μM with a LOD of 0.12 μM, RSD ≤ 1.34%, and a recovery range of 98.0–101.3%. When 3-ASA and 5-ASA were mixed in different ratios, the fluorescence showed different colors. The possible mechanism of the interaction between 3-ASA (or 5-ASA) and Ag@BPQD may be ascribed to the generation of excited-state intramolecular proton transfer. To realize convenient detection of 3-ASA and 5-ASA, a Ag@BPQD portable sensing method using cotton swabs were built. The proposed approach provides the detection of 3-ASA and 5-ASA in environmental and biological samples with high efficiency, accuracy and portability. Graphical Abstract
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 49
·期 1
·241-252
·
IF 3.134
Xing Qianqian,Zhao Jiancheng,Zhu Yulei,Hou Xianglin,Wang Yingxiong
5-Chloro-2-pentanone (5C2P) and its derivatives are widely utilized in the pharmaceutical and agrochemical industry. A new catalytic approach was proposed to convert 3-acetyl-1-propanol to 5C2P using bis(trichloromethyl)carbonate (triphosgene, BTC) as the efficient chlorine source. Various qualitative and quantitative nuclear magnetic resonance techniques ( 1 H, 13 C NMR), especially 1D selective gradient total correlation spectroscopy (Sel-TOCSY) and 2D heteronuclear single quantum correlation ( 1 H- 13 C HSQC) were used in the process. The reaction conditions, such as temperature, time, mole ratio, solvent as well as initiator were optimized. Experiment results showed that the yield of 5C2P reached a maximum of 97.93% in 1,2-dichloroethane at 80 °C after 2 h under the initiation of N,N-dimethylacetamide, and the optimal molar ratio of 3-acetyl-1-propanol to BTC was 1:0.4. The reaction mechanism was proposed and confirmed accordingly. Interestingly, an intermediate product of 1-(dimethylamino)ethyl carbonochloridate was observed, and its chemical structure was characterized by both Sel-TOCSY and 1 H- 13 C HSQC. This study enriched the catalytic reaction ways for the preparation of 5C2P.
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2022
·Vol. 69
·期 5
·e17974
·
IF 4.167
Hao Yan,Delun Ren,Zhiqiang Li,Junshu Chen,Xinyang Zhang,Yanhao Wang,Gongzheng Duan,Xiang Feng,Xin Zhou,Yibin Liu,Xiaobo Chen,Chaohe Yang
Engineering acid site spatial location of zeolite catalyst harbors tremendous potential to boost catalytic performance but still remains a grand challenge for aromatization reaction. Herein, we successfully manipulate acid site spatial location inside the ZSM-5 channels to promote the hexane aromatization via the simple SiO 2 coating treatment. Multi-techniques demonstrated that the medium strong L acid in the channel originated from the Si(Al) O Zn structure is mainly retained in the Zn/ZSM-5-Si catalyst by covering the acid sites outside the channel. Surprisingly, there is a good linear relationship between BTEX yield and this medium strong L acid content. Based on the reaction kinetics, in situ FT-IR and theoretical calculations, it is found that the L acid with confinement effect served as the main active site could prominently enhance the cyclization of propene intermediate and the dehydrogenation of cycloalkane due to the strong affinity between the C/H and ZnOx, and control the desorption of BTEX (mainly benzene, toluene, ethylbenzene, and p-xylene) by weakening the binding of hydrogen proton to π electrons. Compared with the ordinary Zn/ZSM-5 catalyst, the yield of BTEX is increased by nearly 10%, and the Zn/ZSM-5-Si catalyst exhibits excellent anti coking deactivation ability. This strategy together with mechanistic results may pave the rational design of efficient Zn/ZSM-5 catalysts for aromatization reaction.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）