Advanced Energy and Sustainability Research
·
2023
·Vol. 4
·期 12
·2300122
·
IF 5.8
Jian Lei,Hongyuan Yang,Ziliang Chen,Sugang Meng,Nan Zhou,Yang Yang,Prashanth W. Menezes
CO 2 reduction (CO 2 RR) with selective benzyl alcohol (BA) oxidation in a single photoredox reaction can simultaneously utilize photogenerated electrons and holes to realize efficient production of fuels and value-added chemicals. Herein, a unique 2D/1D ZnIn 2 S 4 /In 2 O 3 (ZIS/In 2 O 3 ) heterostructure is developed displaying outstanding performance for photoredox catalysis. As is unequivocally illustrated by various advanced ex situ/in situ characterizations and theoretic calculations, the notable catalytic performances originate from the built-in interfacial electric field within the ZIS/In 2 O 3 heterostructure, which strongly ameliorates the separation and transport of charge carriers. Remarkably, the catalytic activity can further be boosted after coupling the additional thermal treatments, and the product selectivity is highly temperature dependent. Thereby, the precise formation of targeted products, which can serve as valuable industrial products and fuels can be controlled by changing the reaction temperatures, including obtaining the syngas with different H 2 /CO ratios from CO 2 reduction, as well as benzaldehyde, hydrogenated benzoin, and dibenzyl ether (never reported for BA during photocatalysis) from the BA conversion. This study offers a constructive and inspiring contribution to reasonably developing photoredox catalysts, which can fully utilize photogenerated electrons and holes, as well as demonstrate how to controllably yield the targeted products by coupling thermo- and photoredox catalysis.
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Luyao Guo,Xiaoyan Liu,Ziang Zhao,Ronghe Lin,Yu Meng,Xinzheng Ma,Yihui Li,Xiaoling Mou,Li Yan,Hejun Zhu,Yunjie Ding
Nanostructured bimetallic Pt–Bi catalysts are designed by defect engineering of N-doped carbons as the hosts. The optimal catalyst delivers good yields (>98%) in the direct oxidation of C5–C9 linear α-alcohols to corresponding fatty acids, significantly outperforming activated carbon-supported benchmarks and rivaling the state-of-the-art systems. A combined kinetic and computational study on n-heptanol oxidation as a model reaction unveils the kinetic and thermodynamic origins of the better performance of the PtBi alloy than neat or Bi-modified Pt(111) surfaces. Structure–performance correlations further identify that the metal particle size, surface Bi/Pt ratio, and strong basicity strongly influence the catalyst performance in alcohol oxidation. The creation of nitrogen defects facilitates the formation of the surface PtBi alloy and brings strong basicity, accounting for the boosted performance. These findings enable a step closer toward the manufacture of valuable fatty acids from abundant coal by coupling the advanced oxidation with the recently piloted higher alcohol synthesis via the Co–Co2C-catalyzed Fischer–Tropsch reaction.
✓ 已验证
产品关联
DOI
高影响因子
Food Chemistry-X
·
2023
·
IF 6.1
Yujie Xu,Yaqin Liu,Jihong Yang,Hui Wang,Hanchen Zhou,Pandeng Lei
Traditional Keemun black tea is also known as Congou black tea (CF). Over the last three decades, three other types of Keemun black tea (Jinzhen, JZ; Maofeng, MF; Xiangluo, XL) made by different processing have been introduced into the tea market. Total CF volatile concentrations ranged from 1666.3 to 2185.7 μg/L, followed by XL (1193.5–1916.1 μg/L), JZ (1058.9–1811.0 μg/L), and MF (987.5–1518.0 μg/L) tea infusions. A total of 79 volatiles in tea infusions was identified by two methods, among which fourteen with OAVs > 1 were identified and OAVs proportion of volatiles with flowery, fruity, or sweet notes to those with other notes differed in four Keemun black teas (CF = 6.58:1, MF = 5.16:1, JZ = 4.04:1, XL = 5.11:1). Phenylethyl alcohol oxidation resulted in phenylacetaldehyde formation which is the characteristic odorant in Keemun black tea. We clearly show that changes in tea processing gives the distinctive aroma to different Keemun black teas.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 34
·e202301948
·
IF 2.1
Hai-Bo Wu,Xian-Tai Zhou,Xiao-Wu Zhou,Yan-Xiong Fang
Graphical Benzoic acid has been proved to be an efficient catalyst for the ring-opening polymerization of ϵ-caprolactone under mild conditions. A monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. It is expected to realize the one-step preparing of poly (ϵ-caprolactone) through the direct aerobic oxidation of cyclohexanone. The development of a feasible industrial method for poly(ϵ-caprolactone) (PCL) preparation is great of significant and challenging. The bulk ring-opening polymerization of ϵ-caprolactone (ϵ-CL) using various organic acid catalysts and benzyl alcohol (BnOH) as the initiator was developed. Benzoic acid (BA) has been proved to be an efficient catalyst for the ROP of ϵ-CL under mild conditions. The conversion of ϵ-CL to PCL was 84.7 % under the optimized reaction conditions, with number-average molecular weight ( M n ) and dispersity (PDI) of 7700 g/mol and 1.25, respectively. Moreover, a monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. Overall, this work is expected to provide a feasible industrial method for the preparation of PCL using benzoic acid as organocatalyst.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiaqing Liu,Jun Wan,Lin Liu,Weijie Yang,Jingxiang Low,Xiaoming Gao,Feng Fu
Aiming to the unwanted photocatalytic hydrogen production systems using sacrifice agents, a well-design S-scheme O-ZnIn 2 S 4 /TiO 2- x heterojunction was fabricated to realize photocatalytic hydrogen production via water reduction coupled with organic oxidative dehydrogenation. As supported by DFT calculations and experimental analysis, owing to the synergistic effect of oxygen defect and doping engineering, a tailored energy band structure alignment with higher redox potentials and larger Fermi level potential difference are achieved, resulting in more efficient S-scheme interface charge transfer and separation efficiency, thus improving the photocatalytic activity of O-ZnIn 2 S 4 /TiO 2- x . The optimal O-ZnIn 2 S 4 /TiO 2- x photocatalyst shows remarkable H 2 and benzaldehyde production rate of 2584.9 μmol g -1 h −1 and 2880.5 μmol g -1 h −1 under visible light, which are 52.5 and 66.4 times as high as those over blank TiO 2 . Interestingly, this coupled reaction system also displays superior H 2 evolution activity compared to sacrificial reagent systems of Na 2 SO 3 /Na 2 S and triethanolamine. Further quenching and EPR experiments reveal that both water and organic molecules provide protons for H 2 production.
✓ 已验证
产品关联
DOI
高影响因子
Biomaterials Science
·
2021
·Vol. 9
·期 9
·3348-3361
·
IF 6.843
Yaomin Zhai,Juan Wang,Liyan Qiu
The in vivo delivery of nanomedicine is severely hampered by the limited enhanced permeability and retention effect (EPR) in tumors. Aiming at overcoming this limitation and achieving high anti-tumor effect of chemotherapeutics, we specially addressed an available strategy from a viewpoint of increasing the drug loading of nano-carriers. Here, we constructed a novel pH-responsive polymersome based on the drug-driven self-assembly of amphiphilic polyphosphazenes PAP containing the ortho ester group ABD and mPEG2000. Due to the non-covalent attractive forces between PAP and doxorubicin hydrochloride (DOX·HCl), DOX·HCl can induce the self-assembly of PAP via embedding itself in the lamella to form vesicles and the subsequent location in the center aqueous chamber of the resultant nano-vesicles, which resulted in the high drug loading content of 35.77 wt%. In addition, with the incorporation of cholesteryl hemisuccinate (CholHS), the premature leakage of DOX·HCl was significantly inhibited under physiological conditions. Meanwhile, the pH-sensitive drug release occurred at pH 5.5 by the advantage of the pH-sensitive biodegradation of ABD in PAP. Consequently, this CholHS-incorporated DOX·HCl-driven PAP vesicle achieved excellent anti-tumor effect with tumor growth inhibition up to 82.4% in S180 tumor-bearing mice. Taken together, our newly developed drug-driven vesicles may promote the development of efficient drug delivery systems for application in cancer therapy.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Engineering
·
2021
·
IF 7.553
Dan-Lei Yang,Dan Wang,Hao Niu,Rui-Li Wang,Mei Liu,Fei-Min Zhang,Jie-Xin Wang,Mei-Fang Zhu
Multifunctional fillers are greatly required for dental resin composites (DRCs). In this work, a spray dryer with a three-fluid nozzle was applied for the first time to construct high-performance complex nanoparticle clusters (CNCs) consisting of different functional nanofillers for dental restoration. The application of a three-fluid nozzle can effectively avoid the aggregation of different nanoparticles with opposite zeta potentials before the spray drying process in order to construct regularly shaped CNCs. For a SiO 2 –ZrO 2 binary system, the SiO 2 –ZrO 2 CNCs constructed using a three-fluid nozzle maintained their excellent mechanical properties ((133.3 ± 4.7) MPa, (8.8 ± 0.5) GPa, (371.1 ± 13.3) MPa, and (64.5 ± 0.7) HV for flexural strength, flexural modulus, compressive strength, and hardness of DRCs, respectively), despite the introduction of ZrO 2 nanoparticles, whereas their counterparts constructed using a two-fluid nozzle showed significantly decreased mechanical properties. Furthermore, heat treatment of the SiO 2 –ZrO 2 CNCs significantly improved the mechanical properties and radiopacity of the DRCs. The DRCs containing over 10% mass fraction ZrO 2 nanoparticles can meet the requirement for radiopaque fillers. More importantly, this method can be expanded to ternary or quaternary systems. DRCs filled with SiO 2 –ZrO 2 –ZnO CNCs with a ratio of 56:10:4 displayed high antibacterial activity (antibacterial ratio > 99%) in addition to excellent mechanical properties and radiopacity. Thus, the three-fluid nozzle spray drying technique holds great potential for the efficient construction of multifunctional cluster fillers for DRCs.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yingtong Zou,Yezi Hu,Andrej Uhrich,Zewen Shen,Baoxiang Peng,Zhuoyu Ji,Martin Muhler,Guixia Zhao,Xiangke Wang,Xiaoxiang Xu
We provide a distinct understanding on the role of oxygen vacancies (OVs) for visible light-triggered aerobic oxidation of alcohols via comparative studies on three kinds of Nb 2 O 5 , i.e., undoped, Ti-doped and Ce-doped Nb 2 O 5 . With benzyl alcohol and 5-hydroxymethylfurfural as representative alcohol substrates, we show that fast alcohol oxidation with high selectivity can be achieved on these doped Nb 2 O 5 containing abundant OVs. However, the functionality of OVs is dependent on the properties of dopants as Ce-doped Nb 2 O 5 exhibits a better performance than Ti-doped one. Investigations indicate that the Ce dopants incur little distortion to the structure of Nb 2 O 5 and induce more accessible OVs than Ti dopants for the dissociative chemisorption of alcohol molecules which supports favorable interfacial electron migration process. The present work not only reveals the difference of oxygen vacancies caused by varied metal doping but provides a unique insight in the relation between OVs structure and photocatalytic alcohol oxidation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Ziqiang Zheng,Ting Wang,Fang Han,Qing Yang,Benxia Li
The development of visible light responsive photocatalysts for simultaneous production of hydrogen (H 2 ) fuel and value-added chemicals is greatly promising to solve the energy and environmental issues by improving the utilization efficiency of solar energy. Herein, the three-component Ni/(Au@CdS) core–shell nanostructures were constructed by the hydrothermal synthesis followed with photodeposition. The intimate integration of plasmonic Au nanospheres and visible-light responsive CdS shells modified with Ni cocatalyst facilitated the generation and separation of electron-hole pairs as well as reduced the overpotential of hydrogen evolution. The Ni/(Au@CdS) photocatalyst exhibited excellent performance toward the selective transformation of benzyl alcohol under anaerobic conditions, and the yields of H 2 and benzaldehyde reached up to 3882 and 4242 μmol·g −1 ·h −1 , respectively. The apparent quantum efficiency (AQE) was determined to be 4.09% under the irradiation of 420 nm. The systematic studies have verified the synergy of plasmonic effect and metal cocatalyst on enhancing the photocatalysis. This work highlights the desirable design and potential application of plasmonic photocatalysts for solar-driven coproduction of H 2 fuel and high-value chemicals.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2021
·Vol. 39
·期 9
·2403-2409
·
IF 6
Xiao Jiang,Na Zhao,Zhibo Li
Main observation and conclusion Substantial progresses have been made toward the development of metal-free catalysts for stereoselective ring-opening polymerization (ROP) of rac -lactide. Yet the discovery of organic catalysts effective at ambient temperature remains a major challenge. Here, the bifunctional H-bonding catalyst SQ-1 containing a basic tertiary amine and squaramide motif proved to be good candidate for the stereoselective ROP of rac -lactide at room temperature, yielding stereoregular polylactide with controlled molecular weights (up to 21.1 kg/mol) and high tacticity ( P i ESC up to 0.88). Furthermore, binary H-bonding catalytic system consisting of squaramides (SQ-2 to SQ-6) and 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) could efficiently promote the ROP of rac -lactide at room temperature within short reaction time. Among them, the most bulky squaramide SQ-2 exhibited the best steroselectivity towards the ROP of rac -lactide without transesterification side reactions during the polymerization process. The resulting polylactides were proved to have controlled molecular weights as high as 22.2 kg/mol and narrow distributions (1.10—1.24).
✓ 已验证
产品关联
DOI
高影响因子
FOOD CONTROL
·
2021
·
IF 5.548
Dandan Qi,Aiqing Miao,Wei Chen,Wenwen Wang,Xiugu He,Chengying Ma
Broken oolong-black tea is an innovative tea in China produced by applying characteristic manufacture crafts of broken oolong tea (bruising) and broken black tea (fermentation) on the manufacture of tea and it has both aroma features of broken oolong tea and broken black tea. The aim of this study is to investigate the differences of the volatile compounds among broken oolong-black, broken oolong and broken black tea made by Huangzhixiang (HZX) and Huangdan (HD) varieties by gas chromatography-mass spectrometry (GC-MS) combined with chemometirc analysis. The results suggested significant differences on both aroma quality and volatile compounds profile of three kinds of tea. Chemometric analysis showed that 47 and 52 differential volatile compounds were identified to distinguish three kinds of teas made by HZX and HD, respectively, and the differences of volatile compounds among the tea samples were mostly quantitatively rather than qualitatively. Besides, compounds with floral and fruity aroma increased in broken oolong-black tea compared with the others, while compounds with green aroma decreased in broken oolong-black tea. Quantitative descriptive analysis of the aroma showed that sweet aroma was a new trait of broken oolong-black tea compared with broken oolong tea while green aroma disappeared compared with broken black tea. Our results provide the theoretical and practical meaning for the application of two characteristic crafts from different tea manufacture on the innovation of tea manufacture.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xiaoli Li,Ting Wang,Ziqiang Zheng,Qing Yang,Can Li,Benxia Li
Developing photocatalysts for coproduction of hydrogen fuel and valuable chemicals is highly desired but still challenging. Herein, Pd-modified defective HNb 3 O 8 photocatalyst (denote as Pd/HNb 3 O 8 -H 2 ) consisting of dispersive Pd sites and abundant surface oxygen vacancies (V O s) was prepared via the thermal treatment of Pd 2+ -incorporated HNb 3 O 8 in H 2 /Ar gas. The existence of Pd favors the formation of V O s on HNb 3 O 8 , enabling the synchronous construction of Pd and V O dual active sites. The spectroscopy and photoelectrochemical studies demonstrate the advantages of Pd/HNb 3 O 8 -H 2 photocatalyst in promoting the separation and migration of photoinduced charge carries. The Pd/HNb 3 O 8 -H 2 photocatalyst exhibits the outstanding performance toward photocatalytic proton reduction coupled with selective benzyl-alcohol oxidation , achieving the optimal production rates of H 2 and benzaldehyde as high as 3.17 and 2.76 mmol·g cat −1 h −1 , respectively. The experimental and theoretical investigations have expounded the synergistic mechanism of Pd and V O dual active sites in boosting photocatalytic coproduction of H 2 and benzaldehyde.
✓ 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）