DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 8
·2392-2403
·
IF 4
Amir Said,Guanyun Zhang,Caiyun Liu,Dexin Wang,Huihui Niu,Yanshu Liu,Guanjie Chen,Chen-Ho Tung,Yifeng Wang
The cycloaddition reaction of CO2 to epoxides is quite promising for CO2 capture and storage as well as the production of value-added fine chemicals. Herein, a novel atomically precise lead-doped titanium-oxide cluster with the formula Ti10Pb2O16(phen)4(Ac)12(DMF)2 (denoted as Ti10Pb2; phen = 1,10-phenanthroline; Ac = acetate; DMF = dimethylformamide) was synthesized through a facile solvothermal process, and is a molecular photocatalyst with surface-anchored main-group metal active sites. Its structure was characterized by single-crystal X-ray diffraction and other complementary techniques. Ti10Pb2 showed high photo-response and charge-separation efficiency under simulated sunlight irradiation. Ti10Pb2 was successfully used in the cycloaddition reaction of CO2 with epoxides under solvent-free conditions. While its catalytic activity due to the Lewis acidity was moderate, simulated solar light irradiation further enhanced the reaction rate, demonstrating the synergistic effect of photocatalysis and Lewis-acid thermocatalysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Song Wang,Yan Wang,Yanchao Zhang,Zhiyan Sui,Junjian Yu,Jialin Zhao,Na Li,Yifang Chang,Di Liu,Zhe Wang
The conformation of N-spirocyclic cations has a high alkaline stability and the construction of microphase-separated structures with poly(biphenyl piperidine) (PBP) is one way to improve the performance of AEM. Here, a variety of N-spirocyclic cations were prepared and formed into polycationic side chains with the PBP main chain via the -(CH 2 ) 4 - spacer group. The ion transport efficiency was greatly enhanced by the synergistic effect of the main chain piperidine cations, and the hydroxide conductivity and peak power density of the MDSU-MPBP membrane reached 132.7 mS cm -1 and 295.2 mW cm -2 at 80 °C, respectively. The BM-DSU cation was degraded to a single cation mainly by the S N 2 reaction after 96 h in a 5 M NaOH/D 2 O solution at 80 °C. The N-spirocyclic mono-cation has extremely high alkali resistance, especially the MDSU cation without significant degradation at 80 °C for 1008 h. The B-MDSU double cation tends to undergo the S N 2 reaction at the C2 and C4 positions. The asymmetrically grafted main-chain piperidine cations exhibit poor chemical stability due to the electron-absorbing effect of the phenyl group. the degradation of the MDSU cations increases the hydrophobicity of the side chains, and the MDSU-MPBP membrane has the best alkali resistance, with a conductivity residual of more than 92.8% after immersion in a 5 M NaOH solution at 80 °C for 480 h.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongyu Niu,Xing-Bao Wang,Jingjie Luo,Jiaxin Liu,Chuang Li,Wen-Ying Li,Changhai Liang
Desulfurization plays a critical role in refining crude oil to produce fuel and the manufacture of fine chemicals. However, its low efficiency becomes a great challenge for the present desulfurization if only the C-S cleavage is considered a promising approach to reducing hydrogen consumption under atmospheric pressure. Accordingly, we investigate the critical factors necessary to achieve high C-S cleavage of dibenzothiophenes under mild conditions of 0.1 MPa and H 2 /oil = 100. The mechanism of reactive adsorption desulfurization of dibenzothiophenes with or without steric hindrance at atmospheric pressure on Pt/ZnO is proposed by studying the adsorption model of active metal sites, the Pt efficiency in C-S cleavage influenced by the steric hindrance and the structural evolution of Pt active centers in the presence of sulfur adsorption/deposition. Based on both experimental and DFT results, we report C-S cleavage of dibenzothiophenes with (TOF = 15 h −1 ) or without steric hindrance (TOF = 128 h −1 ) that can be highly efficiently fractured (99.9%) by the interface between PtS x and ZnO . This work has great practical significance for developing atmospheric industrial adsorbents for ultra-deep reactive adsorption desulfurization.
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL LETTERS
·
2022
·
IF 2.267
Yu Huang,Yi Wu,Wenhui Li,Xiaohui Yan,Dapeng Wu
Highly spherical porous silica particles (PSPs) with a controlled pore size were prepared by ultrasonic spray drying and were used as a packing material for high-performance liquid chromatography (HPLC). By using organic additives added to the silica sol as porogens instead of low-melting salts, choosing the size of the colloidal SiO2 particles, and varying the type and the ratio of additives, the pore size of the PSPs was finely tuned from 2.9 to 34.4 nm. Subsequently, PSPs having pore sizes of 7.4, 13.5, and 29.0 nm were modified by chlorodimethyloctadecylsilane (PSPs-C18), and HPLC columns packed with the different PSPs-C18 were evaluated systematically using aromatic compounds and alkylbenzene derivatives as probes. A plate number of 81,000/m and the relative standard deviation of less than 1% in the retention time were obtained for pentylbenzene over 100 injection and HPLC separation cycles for the 7.4-PSPs-C18 column. Five proteins were also separated within 25 min using the 29.0-PSPs-C18 column.
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Amir Said,Caiyun Liu,Chang Gao,Dexin Wang,Huihui Niu,Yanshu Liu,Guo Wang,Chen-Ho Tung,Yifeng Wang
The CO2 cycloaddition to epoxides is an efficient method for CO2 capture and storage, important not only for reducing greenhouse gas emission but also for producing cyclic carbonates, which are valuable industrial materials. In this study, we report a novel high-nuclearity titanium oxide cluster (TOC) inlayed with main-group element Pb2+, H2Ti16Pb9O24(SA)18(DMF)10(OH2)2 (denoted as 1; SA = salicylate; DMF = N,N-dimethylformamide), which has the property of visible-light absorption and has shown high catalytic activities for cycloadditions of CO2 under visible-light irradiation. The cluster was synthesized in a high yield in a facial solvothermal process. Its structure and electronic structure were characterized by single-crystal X-ray diffraction, density functional theory calculations, and complementary techniques. The cycloaddition reactions were performed under solvent-free conditions. While the catalytic activity due to the Lewis acidity was moderate, visible-light irradiation further folded the reaction rates. The turnover number reached 3400 with a turnover frequency of 120 h–1. Mechanism studies indicated a synergistic effect of the Lewis acidity and photogenerated charge carriers. The performance of 1 in reversible I2 uptake was also investigated. This study demonstrates the high potential of heterometal-decorated TOCs in the cost-effective and efficient CO2 cycloaddition reaction under mild conditions.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Dexin Wang,Amir Said,Yanshu Liu,Huihui Niu,Caiyun Liu,Guo Wang,Zhaoyang Li,Chen-Ho Tung,Yifeng Wang
The solvothermal reaction of titanium isopropoxide and chromate in the presence of benzoate produced two novel host–guest clusters encapsulating Cs+ or H3O+, (H3O)@Ti7Cr14 and Cs@Ti7Cr14. The most remarkable feature is that the Ti7O7 ring is concentrically embraced by a Cr14O14 ring to form a rigid Ti7Cr14 host. ESI-MS and 133Cs NMR revealed that the overall framework structures are preserved, whereas the benzoate ligands on the two clusters may be labile in solutions. Both (H3O)@Ti7Cr14 and Cs@Ti7Cr14 exhibit good UV–vis light-responsive properties and photocatalytic activities, with absorption edges extending up to 780 nm. Cs@Ti7Cr14 is an effective visible-light-responsive photocatalyst in both the heterogeneous methylene dye degradation and homogeneous CO2 cycloaddition reaction under mild conditions like room temperature and 1 bar of CO2. According to the mechanism studies, Cs+, as a rigid guest, can significantly improve the photogenerated charge separation efficiency of the Ti7Cr14 host, thereby improving its interface charge separation properties, photocurrent, and photocatalytic activities. Our findings not only provide new members of heterometallic titanium oxide clusters to enrich the metal oxide cluster family but also open up new possibilities for their photoresponses, which may play an important role in solar energy harvesting for sustainable chemistry.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MACROMOLECULES
·
2022
·
IF 6.057
Xiaofeng Li,Kuan Yang,Zimo Wang,Yaohan Chen,Yonggang Li,Jing Guo,Jifu Zheng,Shenghai Li,Suobo Zhang
Main-chain non-ether anion-exchange membranes (AEMs) have become a research hotspot in recent years because of their ease of preparation and excellent alkaline stability. However, owing to the limitations of the types of monomers and polymerization mechanisms, preparing main-chain non-ether AEMs with controllable morphology remains challenging. Herein, seven poly(fluorene alkylene) membranes, including random and block-structured membranes with different quaternary ammonium (QA) group distributions on the side chains, with the same ion-exchange capacity (IEC) were designed via superacid-catalyzed polymerization. The properties of the as-synthesized membranes were characterized, and the water-transport mechanism has been discussed in relation to the morphology of the membranes. The formed bicontinuous phase structure based on block biphenyl units possessed multidirectional ion channels and distinct ion clusters favorable to water molecule movement. The conductivity of the optimized membrane with a block biphenyl structure reached 208 mS cm–1 at 80 °C, and the peak power density of an H2/O2 fuel cell based on the as-prepared membrane was 0.92 W cm–2. The reported approach is effective in balancing the content of free and bound water within the membrane, generating maximum hydroxide mobility and water transport suitable for high-performance AEM fuel cells. This study highlights the significance of regulating the block structure and adjusting the segment distribution in AEMs to tune their morphologies and provides an innovative design approach for constructing high-performance AEMs.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Qiao Liu,Wenli Ma,Lin Tian,Junmin Li,Lincan Yang,Fanghui Wang,Zhiqian Wang,Jing Li,Zhongming Wang,Hong Zhu
To achieve high-performance anion exchange membranes (AEMs) with superior conductivity and stability, a series of novel poly(biphenyl piperidinium) (PBP-n-Pip) membranes are synthesized by tethering cationic groups to the backbone utilizing flexible hydrophobic alkyl spacers with various lengths. All of the membranes exhibit excellent film-forming ability and tensile strength (42.34–53.49 MPa). Well-defined microphase separation is confirmed by transmission electron microscopy (TEM) and atomic force microscopy (AFM). The PBP-6-Pip membrane exhibits the conductivity of 117.1 mS cm −1 at 80 °C due to the most excellent microphase-separated morphology and highest water uptake. The long-term alkali resistance of AEMs can be improved by extending the length of the flexible alkyl chains appropriately. After immersion in 2 M NaOH at 80 °C for 1500 h, the initial conductivity of PBP-6-Pip with intermediate spacer chains and PBP-8-Pip with longer spacer chains both remains above 84%. Furthermore, the PBP-6-Pip membrane with the highest conductivity achieves a peak power density of 307 mW cm −2 at 80 °C in the H 2 /O 2 single fuel cell. A long-term life test of this MEA shows a voltage decay rate of 2.87 mV/h over 40 h of operation under 0.2 A cm −2 at 60 °C.
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Bo Tang,Di Wang,Ang Li,Hui-Min Tang,En-Cui Yang,Weili Dai
Herein, core-shell structured Snβ@mesosilica (MS) composite was constructed by oriented assembly of mesoporous silica on microporous Snβ zeolite . The mesoporous channels in the shell were verified vertically aligned to the Snβ core, rendering sufficient mass transfer between the shell and core. The resultant Snβ@MS was thereafter employed as the scaffolds for anchoring Au nanoparticles to develop a bifunctional Au/Snβ@MS catalyst for one-pot base-free conversion of glycerol to methyl lactate (ML), which is regarded as a promising and sustainable route to ML production. Under optimum reaction conditions, a remarkable activity with 98.2% glycerol conversion and 91.9% ML selectivity was achieved. More importantly, the introduction of mesoporous silica shell can efficiently modify the Lewis/Brønsted acid ratio of Snβ@MS, thus inhibit the side reactions. While the confinement effects could protect the highly dispersed Au nanoparticles against sintering. Accordingly, a high stability and recyclability was achieved over the Au/Snβ@MS catalyst.
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy and Sustainability Research
·
2022
·Vol. 3
·期 10
·2200083
·
IF 0
Shiming Chen,Zijian Wang,Lu Wang,Zhibo Song,Kai Yang,Wenguang Zhao,Lele Liu,Jianjun Fang,Guoyu Qian,Feng Pan,Luyi Yang
Being considered as a promising anode material for next-generation lithium-ion batteries, silicon oxide (SiO x ) suffers from low initial coulombic efficiency and unstable solid–electrolyte interphase (SEI), which hinder its commercial use. To address these issues, herein, an optimized chemical prelithiation method is developed using a molecularly engineered lithium–biphenyl-type complex, which facilitates improved prelithiation efficiency. More importantly, owing to the reaction between the prelithiation agent and sodium carboxymethyl cellulose binder, a stable artificial SEI layer with hard inorganic particles embedded in soft organic matrix can be preformed on the surface of the SiO x anode after prelithiation. The preformed SEI layer remains stable during long-term cycling, contributing to significant improvement of capacity retention (87.4%) over pristine SiO x (68.6%) after 100 cycles at 0.2 C. Through demonstrating a hitherto unknown interfacial constructing strategy for SiO x , this study provides a fresh perspective on realizing high-capacity Si-based anodes.
✓ 已验证
产品关联
DOI
ACS Applied Nano Materials
·
2022
·
IF 6.14
Fan Yang,Hongbo Yu,Chunzheng Wu,Shiwei Wang,Tong Li,Hongfeng Yin
Supported Rh nanoparticles (NPs) exhibit excellent activity for the chemoselective hydrogenation of halonitrobenzenes (HNBs), but their selectivity to aromatic amines is not satisfactory due to the side reaction on the carbon–halogen bonds, and their recycling stability is limited due to the aggregation and the leaching of active component during the long-term usage. Herein, we design a yolk–shell-structured catalyst that consists of RhCu alloy cores and hollow/microporous carbon shells (HCS) to overcome these problems. The obtained RhCu@HCS catalyst with a Rh/Cu ratio of 1:1 showed good activity, selectivity, and stability in the hydrogenation of p-CNB (p-chloronitrobenzene) to produce p-CAN (p-chloroaniline) due to the synergistic effect between Rh and Cu. The protective carbon shells not only prevented the aggregation of metal NPs but also allowed the reactants to diffuse freely across the shells. Therefore, our research provides a general strategy to design highly efficient and stable hydrogenation catalysts.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2022
·
IF 5.907
Jiangtao Peng,Ruifeng Guo,Xiongxi Shi,Peiping Zhang,Fagui Qiu,Wenqing Li,Cundi Wei,Shiding Miao
A type of clay-supported catalysts was developed for cycloaddition of CO 2 by immobilizing metal-free ionic liquids (IL) on ball clay (BC) via a one-step strategy. The metal-free IL was loaded on the surface of BC via thermal and acid treatment. The synthesized materials (IL@P-BC) were characterized by Fourier transform infrared spectroscopy (FTIR), N 2 adsorption-desorption, and transmission electron microscopy (TEM). The composite IL@P-BC demonstrated excellent catalytic performance (yield 94.0%, selectively >99%) for coupling of CO 2 with epoxides to produce cyclic carbonates under the lack of any co-catalyst. The good recyclability and excellent suitability were obtained for the composite IL@P-BC. These experimental analyses deepen comprehension of the rational design of clay-based catalysts for CO 2 cycloaddition, further confirmed ball clay was a promising support.
✓ 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）