Materials Horizons
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2023
·Vol. 11
·期 3
·768-780
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IF 13.3
Guiyang Yu,Ke Gong,Xiang Li,Luyang Guo,Xiyou Li,Debao Wang
The achievement of dual-functional photocatalytic technology requires a photocatalyst with accelerated charge flow and purposeful active-site arrangement. In this study, we developed an oriented embedding strategy to induce ReS2 growth at the S vacancy in twin-crystal Zn0.5Cd0.5S solid solution (Sv-ZCS), obtaining an atomic-level heterostructure (ReS2/Sv-ZCS). The electronic structure calculations demonstrate that the charge density of the Zn atom around the S vacancy is higher than for other Zn atoms and the introduced S vacancy establishes a high-speed channel for electron transport via formed Zn–S–Re bonds at the interface between ReS2 and Sv-ZCS. Photogenerated electrons and holes gathered on Re atoms and Sv-ZCS, respectively, which achieves spatial charge separation and separated arrangement for redox sites. As a result, the optimized ReS2/Sv-ZCS heterostructure possesses high efficiency of electron injection (2.6-fold) and charge separation (8.44-fold), as well as excellent conductivity capability (20.16-fold). The photocatalytic performance of the ReS2/Sv-ZCS composite exhibits highly improved dual-functional activity with simultaneous H2 evolution and selective oxidation of benzyl alcohol. The reaction rate of benzaldehyde and H2 evolution reaches 125 mmol gcat−1 h−1 and 159 mmol gcat−1 h−1, which is the highest efficiency achieved so far for simultaneous coproduction of H2 fuel and organic chemicals on ReS2-based composites. This work enriches the application of ReS2-modified composites in a dual-functional photoredox system and also gives insight into the role of defects in electronic structure modification and activity improvement.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia Wu,Ke Wang,Tianqi Yu,Shuaiqin Huang,Zhixiang Zhai,Huan Wen,Shibin Yin
The development of catalysts with high activity, selectivity, and stability is critical for biomass upgrading coupled with hydrogen evolution. In this study, we present a simple method for fabricating crystalline-amorphous phase heterostructures using the etching effect of the acidic medium generated during cobalt salt hydrolysis, resulting in the formation of NiCo(OH) x -modified Ni/NiMoO 4 nanosheets electrode (NiCo(OH) x /Ni/NiMoO 4 /NF). The nanosheets array formed during the synthesis process enlarges the surface area of the prepared catalyst, which facilitates the exposure of electrochemically active sites and improves mass transfer. Unexpectedly, the strong coupling interactions between the amorphous-crystalline heterointerface optimize the adsorption of reaction molecules and the corresponding charge transfer process, consequently boosting the catalytic activity for the 5-hydroxymethylfurfural oxidation reaction (HMFOR) and hydrogen evolution reaction (HER). Specifically, NiCo(OH) x /Ni/NiMoO 4 /NF catalyst requires only 1.34 V to obtain a current density of 10 mA cm −2 for HMFOR-coupled H 2 evolution, and operates stably for 13 consecutive cycles with good product selectivity. This work thus provides insights into the design of efficient and robust catalysts for HMFOR-assisted H 2 evolution.
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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.
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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.
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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.
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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.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Lu Huang,Yingjie Guo,Tianqi Jin,Ke Yan,Xianglin Liu,Shuyang He,Lin Li,Ye Gong,Junyi Ma,Hang Yu,Zhoumin Lu,Yupeng Liu,Wuzi Dong,Fangxia Yang
Triterpene acids (TTAs) have promising applications in functional food, medicine and other fields. Here, ultrasonic-assisted hydrophobic deep eutectic solvent (HDES) extraction was employed to gain TTAs from loquat leaves. Combining COSMO-SAC model prediction with experimental verification，the HDES, composed of thymol and benzyl alcohol (molar ratio 2:1), was proved to have the highest extraction ability for TTAs. The preliminarily optimized extraction conditions were solid to solvent ratio 1:10 (g/g), temperature 60 °C and extraction time 60 min. Under these conditions, the extraction yield of ursolic acid (the main component of loquat leaf TTAs) was 17.769 ± 0.799 mg/g dry loquat leaf. HDES and TTAs were recovered from HDES extracting solution via gradient elution (60% and 80% ethanol aqueous solution, respectively) based on C18 reverse-phase silica gel column chromatography under low pressure (0.5 MPa). Recovered HDES could be reused for extracting TTAs from loquat leaves directly and had a similar extraction performance compared to fresh HDES. The purity of the obtained crude TTAs sample was 81.18% based on the total contents of maslinic acid (MA), corosolic acid (CA), oleanolic acid (OA) and ursolic acid (UA), with a mass ratio of 11:26:10:53. Crude TTAs sample was further separated by C18 reverse-phase silica gel column chromatography using 80% ethanol aqueous solution as mobile phase under high pressure (15 Mpa). By this mean, CA sample with 69.30% purity (MA to CA mass ratio 7:18) and UA sample with 93.94% purity (OA to UA mass ratio 4:21) were obtained. The in vitro antioxidant ability order of the attained TTAs samples was CA sample > crude TTAs sample > UA sample. This study laid a good scientific basis for applying HDES and C18 reverse-phase silica gel column chromatography in the bioactive component extraction and separation fields. It also provided theoretical basis and technical support for obtainment and utilization of high-purity loquat leaf TTAs in the fields of medicine, functional food, cosmetics and so on.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 141
·期 2
·e54774
·
IF 3
Wenyu Zhang,Yu Zhang,Weijie Cai,Dazhi Wang,Shaoyin Zhang
2,2,6,6-Tetramethylpiperidinium-nitroxide (TEMPO) is a mild and efficient catalyst, which is important in the industrial production of selective oxidation of alcohols to the corresponding aldehyde or ketone compounds. However, it is a challenge to recover the expensive TEMPO catalyst in homogeneous catalytic systems. In this study, a novel polymer-supported catalyst was prepared using 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxy (4-OH-TEMPO) and polyaromatic ether sulfone (PAES). The successful grafting of 4-OH-TEMPO in PAES-C was demonstrated by 1 H nuclear magnetic resonance ( 1 H NMR) and Fourier transform infrared (FT-IR), load capacity can be calculated by elemental analysis (EA). BET and scanning electron microscopy (SEM) to depict the structure-performance relationship. Herein, SEM images revealed the existence of porous structure. This structure can effectively adsorb NO molecules to form a PAES-TEMPO/NO x catalytic system to selectively oxidize benzyl alcohol. The experimental results indicated the high activity, the subsequent benzyl alcohol oxidation cycle can reach more than 93% conversion without showing a large loss of selectivity. More importantly, the as-prepared catalyst exhibited the attractive recyclability (recovery rate is 98%). After 10 consecutive runs, no significant loss of conversion and selectivity was observed (the conversion rate of benzyl alcohol was more than 93% and the selectivity was more than 95%). This study might provide some recommendation on the development of highly efficient catalysts for alcohol oxidation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Siyu Ma,Zhihao Wang,Bowen Liu,Xiaolei Wang,Shichao Du,Zichen Song,Xinxin Bian,Manchen Hao,Ju Huang,Zhimin Chen,Zhiyu Ren
Pairing the hydrogen evolution reaction (HER) with the thermodynamics-friendly electrooxidation reaction (EOR) is a powerful way to maximize the energy/economic effectiveness, but still a challenge. Herein, the symbiotic Ni/MoN heterojunction arrays were constructed on foam (Ni/MoN/NF) by the nitridation-induced in situ reduction/conversion strategy. The fascinating interfacial electronic structure and surface reconstruction of Ni/MoN/NF heterojunction are responsible for the enhanced HMF-H 2 O paired electrolysis. Ni/MoN/NF only requires a low overpotential of 53 mV to reach the HER current density of 10 mA cm −2 , as well as the good durability; and NiOOH derived on the anode are electronically activated by MoN to achieving high-efficiency conversion from HMF to FDCA (∼100 % conversion, 97.5 % yield and 97.4 % Faradaic efficiency). For the HMF-H 2 O paired electrolysis, the assembled Ni/MoN/NF||Ni/MoN/NF electrolyzer only requires a low potential of 1.391 V to yield the current density of 10 mA cm −2 , ranking at the forefront in the reported coupling catalysts. Theoretical calculations manifest that the upshift of d -band center of the NiOOH/MoN heterojunction contributes to HMF chemisorption and activation, thereby enhancing its catalytic activity towards HMFEOR. Our study sheds light on the significance of designing the paired electrolysis with low voltage input for renewable energy applications.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Meiqin Li,Zhihui Feng,Fang Wang,Jianxin Chen,Jie Fan,Jieqiong Wang,Zhengquan Liu,Junfeng Yin
There is a huge demand for brewing water in tea consumption, and the sensory flavor of tea infusion is significantly affected by the water used for brewing. To investigate the impact of brewing water on the aroma of tea infusions made from Camelia senensis , the three tea infusions of green, oolong and black tea brewed by six different drinking waters were analyzed by sensory evaluation, solid-phase microextraction, gas chromatography–mass spectrometry, and chemometrics. Brewing water with high pH values (>8.10) and high TDS content (>140 ppm) resulted in a lower overall aroma acceptability for tea infusion, where HCO 3 – , Ca 2+ and Mg 2+ were key influencing ions. A total of 86, 106, and 131 volatiles were identified in green, oolong and black tea infusions, respectively, which were strongly influenced by six different brands of waters. Decanal, dimethyl sulfide, β-ionone and linalool were potent volatiles in tea aroma changes caused by brewing water.
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MACROMOLECULAR RAPID COMMUNICATIONS
·
2023
·Vol. 44
·期 24
·2300371
·
IF 4.6
Shikun Zhao,Shun Gong,Biao Zhao,Like Hou,Lurong Zhang,Qing Hu,Kai Pan
Polyamide 56 (PA56) has gained significant attention in the academic field due to its remarkable mechanical and thermal properties as a highly efficient and versatile biobased material. Its superior moisture absorption property also makes it a unique advantage in the realm of fiber textiles. However, despite extensive investigations on PA56's molecular and aggregate state structure, as well as processing modifications, little attention has been paid to its polymerization mechanism. Herein, the influence of temperature and time on PA56's polycondensation reaction is detailed studied by end-group titration and carbon nuclear magnetic resonance (NMR) techniques. The reaction kinetics equations for the pre-polymerization and vacuum melt-polymerization stages of PA56 are established, and possible side reactions during the polycondensation process are analyzed. By optimizing the reaction process based on kinetic characteristics, PA56 resin with superior comprehensive properties (melting temperature of 252.6 °C, degradation temperature of 371.6 °C, and tensile strength of 75 MPa) is obtained. The findings provide theoretical support for the industrial production of high-quality biobased PA56.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Bing Xing,Ting Wang,Xiaobo Han,Kun Zhang,Benxia Li
The rational integration of semiconductor quantum dots (QDs) with anatase TiO 2 nanostructures is a promising strategy to develop efficient photocatalysts. Herein, Bi 2 S 3 QD/TiO 2 photocatalyst was constructed by controllably depositing Bi 2 S 3 QDs on flower-like TiO 2 nanostructures and used for the photocatalytic redox-coupling reaction of H 2 evolution and oxidative transformation of benzyl alcohol. The abundant amino groups in TiO 2 nanostructures served as the anchoring sites for uniform growth of Bi 2 S 3 QDs. The anchoring of Bi 2 S 3 QDs onto TiO 2 nanostructures not only enhanced the photoabsorption ability and the photogenerated charge separation efficiency but also afforded powerful photogenerated charge carriers and abundant active sites for the photocatalytic reaction. As a result, the Bi 2 S 3 QD/TiO 2 photocatalyst exhibited a favorable performance in the redox-coupling reaction, providing the high production rates of H 2 up to 4.75 mmol·g cat −1 ·h −1 and benzaldehyde up to 6.12 mmol·g cat −1 ·h −1 , respectively, as well as an excellent stability in the long-term photocatalytic reaction. Meanwhile, a trace amount of water in the reaction system could act as a promoter to accelerate the photocatalytic redox-coupling reaction. The photocatalytic mechanism following S-scheme heterojunction was proposed according to the systematic characterizations and experimental results. This work offers some insight into the rational construction of efficient and cost-effective photocatalysts for the conversion of solar to chemical energy.
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