TALANTA
·
2023
·
IF 6.1
Fei Wang,Fan Yang,Jiawei Liu,Quan Bai
This paper is a continuation of research into the retention behavior and mechanism of solutes in hydrophilic interaction chromatography (HILIC) using stoichiometric displacement theory (SDT). A HILIC/reversed-phase liquid chromatography (RPLC) dual-retention mechanism was studied in detail using a β -CD HILIC column. The retention behaviors of three groups of solutes with varying polarities were studied over the entire range of water concentrations in the mobile phase on the β -CD column, resulting in the formation of “U-shape” curves when lg k ’ was plotted against lg[H 2 O]. Additionally, the effect of hydrophobic distribution coefficient lg P O/W on the retention behaviors of solutes in HILIC and RPLC modes was also examined. A four-parameter equation derived from the SDT-R was found to accurately describe the “U-shaped” curves of solutes with RPLC/HILIC dual-retention mechanisms on β -CD column. The theoretical lg k ’ values of solutes calculated using the equation were found to be in agreement with their experimental values, with correlation coefficients greater than 0.99. This indicates that the four-parameter equation derived from SDT-R can effectively describe the retention behaviors of solutes over the entire range of water concentrations in the mobile phase in HILIC. As such, SDT can be used as a theoretical guide for the development of HILIC, including the exploration of new dual-function stationary phases to enhance separation efficiency.
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CHINESE JOURNAL OF CATALYSIS
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2023
·
IF 16.5
Cheng Liu,Mengning Chen,Yingzhang Shi,Zhiwen Wang,Wei Guo,Sen Lin,Jinhong Bi,Ling Wu
Two ultrathin ZnTi-LDH nanosheets with different thickness (1.4 and 4.0 nm) were prepared to study the interplay between the active site and catalytic performance in photocatalytic synthesis of N -benzylideneanilline via a tandem reaction. ZnTi-LDH nanosheet possesses dual isolated active sites including the coordinatively unsaturated Ti atoms (Lewis acid sites) and the H atoms of OH groups (Brönsted acid sites), achieving the activation of benzyl alcohol and nitrobenzene via C–O···Ti species and N–O···H–O species, respectively. Photogenerated holes and electrons facilitate the oxidation of benzyl alcohol to benzaldehyde and the reduction of nitrobenzene to aniline, respectively. The thinner sample possesses more active sites, facilitating not only the activation of reactants but also the separation of photogenerated carriers. Therefore, a thinner ZnTi-LDH nanosheet shows the high conversion (100%) and the high selectivity (96%). Finally, a synergetic photocatalytic mechanism connected to the molecular activation is illustrated at the molecule level.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Xinmiao Li,Kai Deng,Hongjie Yu,You Xu,Hongjing Wang,Liang Wang
The use of thermodynamically more favorable sulfion oxidation reaction (SOR) to replace sluggish oxygen evolution reaction is an effective method for energy-saving production of hydrogen. Herein, we propose the synthesis of organic–inorganic hybrid through the modification of 1-hydroxyethylidene-1,1-diphosphonic acid on Rh metallene (HEDP-Rh metallene) as a bifunctional electrocatalyst for hydrogen evolution reaction (HER) and SOR. The modification of hydrophilic HEDP can effectively promote the water adsorption, thereby accelerating the mass/electron transfer at the interface. The HEDP-Rh metallene requires low overpotentials of 30 mV at 10 mA cm −2 for HER and 0.538 V at 100 mA cm −2 for SOR. In HER-SOR coupled reaction, HEDP-Rh metallene drives the current density of 100 mA cm −2 at 1.08 V for concurrent production of hydrogen and sulfur, highlighting energy-efficient hydrogen production and sulfur recycle.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 19
·5686-5693
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IF 7
Hongjing Wang,Yuqin Liang,Songliang Liu,Xu Mu,Hongjie Yu,Kai Deng,Ziqiang Wang,You Xu,Liang Wang
Coupling the thermodynamically favorable sulfion oxidation reaction (SOR) with the hydrogen evolution reaction (HER) is a promising approach to simultaneously save energy and cost-effectively produce high value-added chemicals and hydrogen. The construction of efficient bifunctional catalysts for SOR–HER electrocatalysis is of significance yet challenging. Here, we propose a dual-nonmetal-doping strategy to construct S and P dual-doped Rh metallene (SP-Rhlene). Benefiting from the combined advantages of dual heteroatom doping and an ultrathin nanosheet structure, SP-Rhlene with a large electrochemical active area and an optimized electronic structure exhibits outstanding HER and SOR activities. A two-electrode system based on optimized SP-Rhlene only needs a cell voltage of 0.385 V at 10 mA cm−2 to generate H2, while transforming S2− into sulfur powder, which further reduces the cost of hydrogen production and protects the ecological environment. This work provides a directive strategy for the rational construction of dual heteroatom doped metallene for energy-saving hydrogen production and environmentally friendly sulfur recovery.
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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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NANOTECHNOLOGY
·
2023
·Vol. 34
·期 35
·355402
·
IF 3.5
Qian Liu,Seng Dong,Yuanzhe Wang,Weiyi Jia,Xi Chen,Faming Gao,Yatao Wang
Fuel cells, as the alternative to fossil energy, have engaged widespread attention by reason of the high conversion efficiency from the chemical energy to the electric energy combined with low pollution emissions. The cathodic ORR catalysts with excellent performance and cost-effectiveness are the dominant point towards the massive development of fuel cells. Here, our group select the Pd NWs as the template and construct the Pd@PtRuNi core–shell bilayer nanostructure to expand platinum atom utilization. Pd@PtRuNi bilayer core–shell NWs unfold elevated mass activity of 1.62\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{metal}}}^{-1} at 0.9 V versus RHE in alkaline media, 2.03- and 6.23-fold of pristine Pd NWs and benchmark commercial Pt/C, respectively. Meanwhile, the cyclic stability tests reveal the excellent durability of Pd@PtRuNi NWs, whose mass activity is only 13.58% degradation after accelerated durability tests. The catalytic activity and durability towards ORR are better than the U.S. 2025 DOE target (0.44\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{pt}}}^{-1} and less than 40% activity attenuation at 0.9 V after 30 000 potential cycles). The elevated catalytic properties can be traceable to the synergism between the ligand effect of Ni and Ru and one-dimensional structure superiority, which optimizes the electronic structure of active sites, promotes the charge transfer and restrains the agglomeration and detachment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yezi Hu,Duoyue Tang,Zewen Shen,Ling Yao,Guixia Zhao,Xiangke Wang
Photocatalytic extraction of uranium from nuclear wastewater and seawater is a highly promising strategy to avoid environmental pollution and effectively recover uranium resources. Herein, we propose a novel strategy of photochemical for efficiently and high selectively extracting uranium from aqueous solution. The excited UO 2 2+ at a suitable pH range were utilized for initiating the formation of hydrogen peroxide, which then directly reacted with UO 2 2+ to form solid studtite (UO 2 )O 2 ∙4 H 2 O. This photochemically triggered extraction approach could remove ∼100.0% of UO 2 2+ from aqueous solution with U(VI) concentration of 10.0–200.0 ppm, and 62.7% of UO 2 2+ from U(VI)-spiked real seawater after 24 hrs-irradiation under visible light even without additional electron-donor agents. The highly selective and high extraction efficiency towards uranium ranged in extremely wide concentrations demonstrated the powerful application potential in both the removal of uranium from nuclear wastewater and the extraction of uranium from seawater. Data Availability Data will be made available on request.
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NANOTECHNOLOGY
·
2022
·Vol. 34
·期 4
·045402
·
IF 3.953
Wenxin Wang,Kai Deng,Qiqi Mao,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Interface engineering of two-dimensional (2D) materials by conductive polymer modification is one of the valid methods to promote hydrogen evolution reaction (HER) performance. Herein, we report a simple and universal strategy for the synthesis of polypyrrole (PPy) modified Rh metallene (Rh@PPy metallene) towards an efficient pH-universal HER. Due to the unique ultrathin 2D metallene structure and the optimized electronic structure between the metallene-PPy surfaces, the as-prepared Rh@PPy metallene not only exhibits excellent HER activity with low overpotentials of 16, 39 and 42 mV in 0.5 M H2SO4, 1 M KOH, and 1 M phosphate buffer solution at current density of 10 mA cm−2, but also displays outstanding stability and durability. This work provides a well-founded pathway to constructe metallene-organic interfaces for various electrocatalytic applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Chaojie Lyu,Jiarun Cheng,Kaili Wu,Jiwen Wu,Ju Hao,Yuanyuan Chen,Huichao Wang,Yunguo Yang,Ning Wang,Woon-Ming Lau,Jinlong Zheng
Transition metal-based electrocatalysts are the promising candidates to substitute noble metal-based catalysts for water electrolysis, owing to its abundant earth reserves and inexpensive fabrication costs. Interface engineering and cation doping engineering are verified as the effective methods to improve the sluggish electrocatalytic performance of transition metal-based electrocatalysts. Here, we synthesized a self-supported heterostructure of Ce doped Co(OH) 2 nanosheets/CoP nanowires on the support of nickel foam (Ce-Co(OH) 2 /CoP/NF) by simple hydrothermal method , low-temperature phosphorization method. The Ce atom doping can lead to lattice distortion and abundant superficial defects on crystal surface, which will generate more active sites and faster charges transformation. The heterointerface between Ce-Co(OH) 2 and CoP also can lead to electronic structure modulation at interface domain, which not can induce much fresh active sites in this area, but can optimize the active sites to the optimal state for superior catalytic activity. Benefitting from these, it only needs the overpotentials of 253 and 56 mV to realize 10 mA/cm 2 for OER and HER under 1 M KOH solution, which is much enhance than single-phased samples. As the bifunctional electrocatalyst for two-electrode system, it merely requires 1.53 V to attain 10 mA/cm 2 in 1 M KOH, and it also exhibits outstanding overall water splitting performance in alkaline natural electrolyte, along with excellent catalytic long-time durability. In addition, the Ce-Co(OH) 2 /CoP/NF-based electrolyzer also could achieve energy-saving hydrogen production, and simultaneously oxidative degradation of organic materials or biomass upgrading at anode under lower voltages. This work paves a novel idea to fabricate high-efficient bifunctional electrocatalysts for energy-saving H 2 production.
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Food Chemistry: Molecular Sciences
·
2022
·
IF 0
Jihong Yang,Hanchen Zhou,Yaqin Liu,Hui Wang,Yujie Xu,Jianqin Huang,Pandeng Lei
Green tea processed from albino tea varieties often has umami taste and fresh aroma. This study identified green teas made from two types of albino tea cultivar, one having the white shoots (called Naibai, NB) and the other having the yellow shoots (called Huangjinya, HJY). Taste compounds analyses showed that galloylated catechins were highly concentrated in HJY green teas, whereas non-galloylated catechins and amino acids were more abundant in NB green teas. CsTA (involved in the catabolism of galloylated catechins) showed high expression in HJY tea shoots, resulting in gallic acid as a precursor for β -glucogallin biosynthesis being abundant in HJY. CsPDX2.1 (responsible for theanine hydrolyzation) had a lower expression level in NB than HJY shoots. Fatty acid–derived volatiles (FADVs), glycosidically bound volatiles (GBVs) and carotenoid–derived volatiles (CDVs) were highly concentrated in HJY green teas, whereas amino acids–derived volatiles were highly concentrated in NB green teas.
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Agronomy-Basel
·
2022
·Vol. 12
·期 11
·2641
·
IF 3.949
Siying Zhao,Yuehan Qiu,Jianning Luo,Wenwen Wang,Haibin Wu,Xiaoxi Liu,Gangjun Zhao,Hao Gong,Xiaoming Zheng,Yujuan Zhong,Xian Yang,Junxing Li
‘Taro-like’ odor is an important economic trait of pumpkin species. The metabolic and molecular bases of this aromatic trait remain largely unexplored. Therefore, in this study, gas chromatography-mass spectrometry, GC-Olfactometry, and RNA-seq technology were used to illuminate the differential volatile compounds, the key volatile compounds, and differentially expressed genes (DEGs) in leaves from two pumpkin samples. Eight volatile compounds, including (E)-2-nonenal, 3-octanol, 2-ethyl-1-hexanol, 1-nonanol, α-terpineol, 2,3-pentanedione, caryophyllene, and 2-acetyl-1-pyrroline, were only detected in the sample with ‘taro-like’ aroma. Moreover, the variable importance in projection scores of all the above eight volatile compounds were >1.0 using PLS-DA analysis. The compounds 2-acetyl-1-pyrroline, 3-octanol, 1-nonanol, and (E)-3,7-dimethyl-2,6-octadienal were identified as the key contributors using GC-Olfactometry analysis. It was determined that 2-acetyl-1-pyrroline might play a significant role in ‘taro-like’ aroma. Furthermore, most of the differential volatile compounds were derived from fatty acids, and the DEGs were also involved in the pathways related to degradation, metabolism, and biosynthesis of fatty acids. Moreover, five genes involved in the accumulation of 2-acetyl-1-pyrroline showed differential expression, and their expression trends were consistent with 2-acetyl-1-pyrroline. This study offers the basis for further studies on the mechanism of ‘taro-like’ aroma in pumpkins.Keywords:pumpkin;‘taro-like’ aroma;volatiles;transcriptome
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 10
·3074-3091
·
IF 2.936
Faizan Muhammad,Saeed Aamir,Song Piao,Zhang Ruirui,Liu Ruixia,Chang Zhi,Wu Liuzhu,Zhang Manyuan
Vanadium phosphorous oxide (VPO) catalysts have been recognized as heterogeneous catalyst for selective oxidation of low-carbon alkanes i.e., n -butane toward maleic anhydride. This process has widely gained attention globally due to its highly selective and cost-effective process. Herein, we employed Cd 0 . 2 Zn 0 . 8 S as a support for the VPO catalyst and evaluated its n -butane catalytic performance. Compared to the unpromoted catalyst (Blank-VPO), a higher n -butane conversion and MA yield were successfully obtained from the promoted catalyst (Cd 0 . 2 Zn 0 . 8 S@VPO). Interestingly, it reduces the byproducts, i.e., CO 2 and CO emission. Characterization methods such as TGA, XRD, EDS, SEM, FTIR, NH 3 -TPD, XPS, TEM, and Raman spectroscopy were used to characterize the Cd 0 . 2 Zn 0 . 8 S, VPO precursor and catalyst. Graphical Abstract
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危险品化学品经营许可证（带存储）