ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Guoxing Liu,Huai Liu,Junhua Zhang,Rui Zhang,Heng Zhang,Yong Sun,Lincai Peng
Catalytic conversion of concentrated carbohydrates and raw biomass into 5-hydroxymethylfurfural (HMF), an important and value-added platform chemical, is highly desirable for industrial applications but challenging. In this work, the tin pyrophosphate-oxide (SnP2O7–SnO2) catalyst has been designed to efficiently produce HMF from various concentrated carbohydrates and raw biomass. Especially, a high HMF yield of 67.8% was implemented over the SPC4 catalyst from concentrated glucose (36 wt %) in a biphasic solvent system of water and methyl isobutyl ketone. Moreover, the SPC4 catalyst disclosed a wide range of universality for converting various concentrated carbohydrates and raw biomass to HMF with satisfactory yields (45.9–79.5%). To the best of our knowledge, this is the first example of accomplishing appreciable HMF yields from carbohydrates and raw biomass at such a high substrate concentration. It has been demonstrated that the superior catalytic performance of the catalyst should originate from its balanced Lewis and Brønsted acidity and superhydrophilicity property. This work invents a highly promising heterogeneous catalyst for efficiently valorizing renewable lignocellulose-related compounds into versatile furans.
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Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Yunlei Zhang,Bing Li,Yanan Wei,Changhao Yan,Minjia Meng,Yongsheng Yan
Developing a green and economically viable approach for the direct synthesis of metal-organic frameworks (MOFs) catalysts with multifunctional active sites remains the key step for their applications in heterogeneous catalysis field. Herein, we report a green (aqueous solutions), mild (90 °C, atmospheric pressure), and modulated hydrothermal (MHT) approach to synthesize UiO-66-type MOFs catalysts with acid–base bi-functional sites, which were obtained via the coordination of monosodium 2-sulfoterephthalate and 2-aminoterephthalic with zirconium (Zr) ions. More importantly, a series of acid, base and acid–base catalysts with varied acid–base strengths can be readily prepared, by simply varying the ratio of organic ligands for preparing MOFs. The synthesized catalysts were characterized and their performances in glucose dehydration to produce 5-hydroxymethylfurfural (5-HMF) have been evaluated. The developed approach in this work has clearly depicted a roadmap for the facile synthesis of MOFs catalysts to facilitate their potential use in acid–base catalysis.
研究领域:
化学工程
·
催化科学
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FUEL PROCESSING TECHNOLOGY
·
2022
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IF 8.129
Shiyun Mu,Kai Liu,Hong Li,Zhenyu Zhao,Xiaoqi Lyu,Yilai Jiao,Xingang Li,Xin Gao,Xiaolei Fan
This work presents an efficient method of supporting zirconia (ZrO 2 ) on COOH functionalized multi-walled carbon nanotubes (ZrO 2 /MWCNTs(C)) via a microwave (MW)-assisted method, which can be used as an efficient catalyst for converting fructose to 5-HMF. The developed composite by the MW-assisted route shows highly dispersed ZrO 2 with small sizes of 4–5 nm on the carbon support, which could not be achieved the conventional hydrothermal synthesis. Characterization shows a unique zirconia amorphous structure which was ascribed to the special interaction between the carbon support and MW irradiation. Specifically, MWCNTs were heated selectively due to their strong MW-absorbing ability, which led to the formation of microscopic “hot spots”, enabling rapid synthesis (8 min) of highly dispersed ZrO 2 with smaller sizes on the hot surface of MWCNTs. Conversely, under conventional heating, the nucleation rate of ZrO 2 was slow and prone to form agglomerated particles on the carbon support. The amorphous ZrO 2 contributed to the excellent activity of ZrO 2 /MWCNTs(C) in fructose conversion to 5-HMF. In detail, fructose conversion and 5-HMF yield were achieved at ~72.8% and ~62.9%, respectively, for the catalyst prepared by the MW method, whilst they are only about 24.7% and 15.7% over the catalyst prepared by the conventional hydrothermal synthesis.
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BIORESOURCE TECHNOLOGY
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2026
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IF 8.2
Wen Wang,Jinsong Sun,Jiajun Liu,Zihao Zheng,Yaxu Sun,Yongzhuang Liu,Qinqin Xia,Zhihan Tong,Haipeng Yu
ZnCl 2 /H 3 PO 4 combines H-bond disruption and synergistic Brønsted/Lewis acid catalysis for glycosidic bond cleavage. • Cellulose is hydrolyzed to glucose in 10 min with a 94.8 mol% yield and 130 mg/mL concentration. • Solvent shows promise for converting glucose to 5-HMF without solid catalysts or energy-intensive pretreatments. Glucose and 5–hydroxymethylfurfural (5–HMF) are attractive platforms for sustainable biomass valorization, yet cellulose conversion remains limited by substrate concentration, reaction conditions, and complex catalyst designs. Here, we report an acidic bifunctional solvent system (ZnCl 2 –H 3 PO 4 ) that can both disrupt cellulose structure and promote rapid in situ cascade hydrolysis to glucose and 5–HMF. In this system, ZnCl 2 (a Lewis acid) facilitates protonation of the β–1,4–glycosidic oxygen, while H 3 PO 4 (a Brønsted acid) accelerates Zn 2+ desolvation, together reducing cellulose crystallinity, activating C–O–C bonds, and lowering the energy barrier for carbocation formation. Under mild conditions (65°C), the process reaches completion within 10 min, achieving 94.8 mol% glucose (with a high concentration ∼ 130 mg/mL). Furthermore, this bifunctional solvent shows promise for converting the released glucose into 5–HMF by leveraging ZnCl 2 for isomerization and H 3 PO 4 for dehydration. This approach avoids the high temperatures and elaborates catalyst architectures typical of conventional acid hydrolysis, offering a streamlined route to efficient cellulose conversion. Download: Download high-res image (150KB) Download: Download full-size image
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JOURNAL OF NANOPARTICLE RESEARCH
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2023
·Vol. 25
·期 11
·1-12
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IF 2.5
Li Fangyuan,Yao Niu,Yuan Huiyu,Cui Junyan,Jia Quanli
The redox properties of electrode materials play a vital role in electrochemical performance. Fabrication of electrode materials with multiple oxidation species is highly desired for ultrasensitive glucose sensing. Herein, multivalent Cu/Cu 2 O/CuO/C (Cu/C) nanocomposites were successfully prepared for non-enzymatic glucose sensing by in situ pyrolysis of Cu metal-organic framework (Cu 3 (BTC) 2 ·3H 2 O, Cu-BTC) at a critical temperature. Structure characterizations showed that the nanocomposites maintained the original morphology of Cu-BTC crystals and exhibited mesoporous structures. Meanwhile, multiple Cu species containing Cu, Cu 2 O and CuO were generated simultaneously, which were tightly pinned on the ligand-derived carbon layers. Thus, under the synergistic effect of multivalent Cu species, mesoporous structure and intense interface contact, the sensing platforms based on Cu/C nanocomposites exhibited good glucose detection performance with a wide linear range of 0.005-2.0 mM, ultrasensitivity of 147.65 μA mM -1 cm -2 , low detection limit of 6.31 μM (S/N = 3), and favorable anti-interference properties and stability. Especially, the Cu/C sensing platform showed excellent recoveries of glucose when used to monitor glucose in real sample of honey. The good electrochemical activities of Cu/C nanocomposites render them promising candidates for sensors and other applications. Graphical abstract
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Guo-Qi Zhang,Wei-ping Liu,Yu-Han Shi,Yu-Xian Zou,Li-Yao Xu,Hui-Ling Cheng,Tao Wang,Wen-Bin Li,Yan Zhao,Zhi-Hong Xu
In the post-COVID-19 pandemic, the stockpiling of medicines by most households could pose a pollution risk as they may expire over time. In this study, an expired amoxicillin act as carbon source to prepare peroxide-like functional carbon dots nanozymes doped Fe (Fe-CDs). Importantly, a high-value treatment technique for expired drugs was proposed. To obtain outstanding catalytic performance, compared with other commonly doped metals, Fe-CDs catalyzed the oxidation of TMB by H 2 O 2 with the highest efficiency. In particular, the oxidation product of TMB (oxTMB) would be alleviated in the presence of antioxidants. Significantly, antioxidants could briefly cause the fading of oxTMB and the fading level was correlated with various concentrations of antioxidants. Importantly, a sequential injection strategy was introduced to control the fading process caused by antioxidants to improve the accuracy. Under the optimum condition, the limit of detection (LOD) was 0.13 mg/L (for ascorbic acid) with the linear concentration range from 0.5 to 15 mg·L −1 . Finally, the total antioxidant capacity (TAC) in human serum samples were evaluated successfully.
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Zhuoran Wang,Wenjia Li,Zhou Zhang,Lili Jia,Jia Wang
The hydrogenolysis of glucose to 1,2-propylene glycol (1,2-PG) has become a powerful and practical approach to using biomass resources. A series of Pt (2%)/WOx (7.5%) catalysts supported on different kinds of γ-Al2O3 were prepared by stepwise incipient wetness impregnation. The effects of Al2O3 supports on the physicochemical parameters and catalytic capabilities of catalysts used in the hydrogenolysis of glucose to 1,2-PG were investigated. Subsequently, an attempt was made to relate the catalytic activities to the structures of the W species. When Nano-Al2O3 was used as the support, the Pt/WOx/Nano-Al2O3 catalyst demonstrated the best performance, yielding 55.8% 1,2-PG after heating at 245 °C for 1 h. The excellent performance of the Pt/WOx/Nano-Al2O3 catalyst was attributed to the high dispersion of the Pt center and the optimal W species structure on the catalyst surface (monodisperse W species coexisting with the polymerized W species).
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Molecular Medicine Reports
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2023
·Vol. 29
·期 1
·1-17
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IF 3.4
Yao Zhao,Mirensha Yakufu,Chong Ma,Baicai Wang,Jianhua Yang,Junping Hu
Nonalcoholic steatohepatitis (NASH) is emerging as the primary driver of liver disease‑induced fibrosis. The imperative need for noninvasive biomarkers to ascertain disease progression stage is evident. The present study elucidated the biological roles of hub genes that could potentially serve as diagnostic markers for NASH. Using an in vivo approach, C57BL/6J mice were subjected to a high‑fat and fructose diet (HFFD) for 6, 10, 14, 18 or 22 weeks. Serological biochemical indices were assessed and liver specimens were obtained to identify potential markers linked to the NASH process, employing a comprehensive strategy that combined transcriptomic and histopathological analyses. The HFFD regimen induced hyperlipidemia, obesity and insulin resistance, progressively culminating in NASH with fibrosis over time. The transcriptomic analyses indicated temporal patterns of pivotal gene sets intricately connected to NASH progression, which encompassed processes such as glucose homeostasis, inflammatory responses, reactive oxygen species‑mediated damage, lipid metabolism disruptions and the formation of fibrotic tissue. Among these genes, Serpine1 and Mmp9 demonstrated promising diagnostic potential for NASH, with their intrahepatic mRNA expression levels serving as robust indicators. Moreover, the levels of PAI‑1 (encoded by the Serpine1 gene) and MMP‑9 in the serum of mice demonstrated a parallel increase with the duration of HFFD intervention. In vitro experiments utilizing HepG2 cells further validated these findings, demonstrating a significant elevation in the protein expression levels of both PAI‑1 and MMP‑9 upon exposure to free fatty acids, in agreement with the results of the animal study. Consequently, PAI‑1 and MMP‑9 are promising noninvasive biomarkers for assessing the progression of NASH.
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PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2023
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IF 7.4
Zhanpeng Ren,Jianying Wang,Chenglong Xue,Minghua Deng,Haiyang Yu,Tianci Lin,Jiayuan Zheng,Rongxiang He,Xianbao Wang,Jinhua Li
A new type of carbon dot (CD)-functionalized solution-gated graphene transistor (SGGT) sensor was designed and fabricated for the highly sensitive and highly selective detection of glutathione (GSH). The CDs were synthesized via a one-step hydrothermal method using DL-thioctic acid and triethylenetetramine (TETA) as sources of S, N, and C. The CDs have abundant amino and carboxyl groups and were used to modify the surface of the gate electrode of SGGT as probes for detecting GSH. Remarkably, the CDs-SGGT sensor exhibited excellent selectivity and ultrahigh sensitivity to GSH, with an ultralow limit of detection (LOD) of up to 10–19 M. To the best of our knowledge, the sensor outperforms previously reported systems. Moreover, the CDs-SGGT sensor shows rapid detection and good stability. More importantly, the detection of GSH in artificial serum samples was successfully demonstrated.
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Polymers
·
2023
·Vol. 15
·期 21
·4235
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IF 5
Mingyu Guo,Chengfeng Zhou,Yuandong Cui,Wei Jiang,Guangting Han,Zhan Jiang,Haoxi Ben,Xiaoli Yang
The catalytic conversion of cellulose to lactic acid (LA) has garnered significant attention in recent years due to the potential of cellulose as a renewable and sustainable biomass feedstock. Here, a series of Au/W-ZnO catalysts were synthesized and employed to transform cellulose into LA. Through the optimization of reaction parameters and catalyst compositions, we achieved complete cellulose conversion with a selectivity of 54.6% toward LA over Au/W-ZnO at 245 °C for 4 h. This catalyst system also proved effective at converting cotton and kenaf fibers. Structural and chemical characterizations revealed that the synergistic effect of W, ZnO, and Au facilitated mesoporous architecture generation and the establishment of an adequate acidic environment. The catalytic process proceeded through the hydrolysis of cellulose to glucose, isomerization to fructose, and its subsequent conversion to LA, with glucose isomerization identified as the rate-limiting step. These findings provide valuable insights for developing high-performance catalytic systems to convert cellulose.Keywords:cellulose conversion;lactic acid;reaction mechanism;rate-limiting step
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yuqi Liu,Fuyan Kang,Chunyu Bi,Junming Shi,Guoyang Gao,Yulong An,Zhanhua Huang
The simultaneous reforming of biomass into high value-added chemicals and H 2 production by water splitting in a green and environmentally clean way is a very challenging task. Herein, we demonstrate the design of bifunctional Mn x Cd 1-x S photocatalyst with a controllable band gap by bandgap engineering. Bandgap engineering effectively regulates the oxidation and reduction capacity of materials. The design of photocatalysts with suitable conduction bands and valence bands makes the targeted conversion of xylose possible. Innovative conversion of xylose to glyceric acid, lactic acid, and propanoic acid. The optimized Mn 0.7 Cd 0.3 S catalyst showed excellent performance in the production of H 2 (14.06 mmol·g cat -1 ·h −1 , 29.9 times more than CdS and 351.5 times more than MnS), xylose conversion (90%), and C3 organic acid yield (59.2%) without cocatalyst and any scavengers under visible light irradiation. This work shows that a rational photocatalyst design can achieve efficient simultaneous production of high value-added chemicals and clean energy.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Shichao Ma,Xichen Yuan,Xu Yin,Yang Yang,Li Ren
Glucose redox is the indispensable method for biological energy supply, and its concentration in the organism is one of the most vital determinants of its health status. Nevertheless, nearly 10,000 organic substances that coexist with glucose in the blood hinder the glucose detection. As a result, developing a detection method that can feature high sensitivity and selectivity is extremely indispensable. In this work, a silver nanowire aerogel (AgNW-gel) was prepared for non-enzymatic glucose detection. The unique porous structure of aerogel and the high electrical conductivity of silver guarantee rapid electron transport and transfer. Furthermore, the presence of massive mesopores in AgNW-gel imparts high specific surface area which provides a large number of active sites. Compared to enzymatic glucose methods, the AgNW-gel, which is a non-enzymatic assay, has a lower environmental dependence. With the help of these characteristics, the glucose non-enzymatic sensor exhibits a high sensitivity of 1940 μA·mM −1 · cm −2 , a wide linear range from 1.0 to 3.5 mM, and a detection limit of 0.8 mM· cm 2 . In addition, the largest interference signal was only 4.4% of the glucose signal in the interference test for the five common interferents in blood.
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