CATALYSIS LETTERS
·
2024
·Vol. 155
·期 1
·1-17
·
IF 2.3
Wei Ruiping,Wang Ziqi,Yao Mingzhu,Xia Rongying,Liu Huijun,Yang Lei,Ma Guanghui,Gao Lijing,Xiao Guomin
The metal-organic frameworks (MOFs) with oxidative and acidic active sites demonstrate promising potential for tandem reactions involving olefin oxidation carboxylation. In this study, M-BTCs were synthesized via a solvothermal method, employing 1,3,5-benzenetricarboxylic acid (H 3 BTC) as a ligand in combination with various metals (Mn, Co, Cu, Ni). The good thermal stability and morphology of M-BTC was verified by various characterization techniques, and its catalytic performance was evaluated for oxidative carboxylation. The catalytic activity of Mn-BTC, with Mn 3+ / Mn 2+ as the primary oxidation site, was found to be superior in both olefin epoxidation and CO 2 cycloaddition. The effects of reaction conditions on both epoxidation of styrene and the cycloaddition reaction were investigated, respectively. Under optimal reaction conditions (epoxidation: 10 wt% Mn-BTC of styrene, 80 ℃ for 12 h; cycloaddition: 100 ℃ for 12 h with a CO 2 flow rate of 15 ml/min and tetrabutylammonium bromide (TBAB) amount of 15 mol%), a 53% yield of styrene carbonate (SC) was obtained in the assisted tandem reactions. Furthermore, cycling experiments as well as XRD and FT-IR spectra of the catalysts after use demonstrated that Mn-BTC maintained its crystal structure and retained a yield of 49% SC after three cycles. Finally, a possible mechanism for assisted tandem catalytic reaction over Mn-BTC was proposed. Graphic
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Energy Storage Materials
·
2024
·
IF 18.9
Dengxu Wu,Jian Peng,Zhiwen Jiang,Lei Zhu,Yujing Wu,Chang Xu,Zhixuan Wang,Ming Yang,Hong Li,Liquan Chen,Fan Wu
Lithium-metal batteries with solid electrolytes (SEs) have emerged as promising electrochemical energy storage devices due to high energy density and safety. However , inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their practical application. Herein , a new type of room-temperature liquidous Li metal arene complex—Li-Phenanthrene (Phen)-Ether is explored to enable a 3D LiSi@Li-Phen-Ether (3D LSLL) anode with low cost, high safety and high ion/electron-conductivity. Symmetric cells with sulfide SE and 3D LSLL anode deliver an ultra-high critical current density (> 13 mA cm −2 ) and long cycle life (> 1000 h, 0.25 mA cm −2 ). Moreover, full battery (LFP/sulfide SE/3D LSLL) can operate at low-external pressure (0.5 MPa) and ambient temperature by introducing a flexible cathode/sulfide interlayer with high ion conductivity (2 mS cm −1 ). This unprecedented battery configuration demonstrates high-rate (2C) performance and long cycle life (over 300 cycles), which exceeds preciously-reported sulfide SE/lithium batteries at low stack pressures, and may open up a promising route for high-energy-density, cost-effective and safe rechargeable lithium batteries.
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ACS Applied Polymer Materials
·
2025
·
IF 4.7
Xunwang Tang,Zongxue Yu,Junlei Tang,Guangcheng Yang,Xiuzhu Zhang,Yu Chen,Jiajia Hou,Jianjun Wu
As the core component of water electrolysis, anion-exchange membranes (AEMs) necessitate high ionic conductivity, favorable dimensional stability, and chemical stability. Nevertheless, the current generation of AEMs remains inadequate for achieving both high ionic conductivity and long-term chemical stability. The side-chain strategy has been demonstrated to be an effective approach for enhancing the conductivity and durability of AEMs. In order to achieve this objective, a series of poly(aryl piperidine) AEMs were designed, featuring hydrophilic cationic side chains and noncationic alkyl chains, with the aim of investigating the impact of grafting different noncationic side chains on membrane properties. In particular, the PTBPA–BMB–OH membrane displayed favorable OH– ionic conductivity (108.3 mS cm–1 at 80 °C) and satisfactory water uptake and swelling rates of 82.3% and 24.9%, respectively. Moreover, an AEMWE based on PTBPA–BMB–OH membranes exhibited a current density of 467 mA cm–2 (1 M KOH solution, 2 V, and 60 °C). The results indicate that this side-chain structural strategy is an effective method to improve the ionic conductivity and dimensional stability of membranes and shows some potential for application in the field of AEMWE.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Runde Yang,Chong Xie,Xing Wan,Haorong Li,Liangyao Ge,Xiaofeng Li,Guanglei Zhao
cellulose II beads@covalent triazine frameworks (CBCs) are prepared by in situ growth of ultra-dispersed covalent triazine frameworks (CTF) using unmodified regenerated cellulose beads (CBs) as templates. The CBCs as a whole are three-dimensional structures consisting of a layered pore structure and a continuous ultrathin CTF, which combines a functional surface with highly efficient mass transfer. The thickness of the CTF in the prepared CBCs can be controlled at 32–83 nm, which enables the CBC to have a dye adsorption efficiency of up to 191 mg g −1 and an ultrafast dye removal time (Methylene Blue, 0.5 min, 95 %). Molecular dynamics simulations revealed the mechanism for CTF growth on the surface of unmodified cellulose II rather than on the surface of cellulose Ⅰ, and the effects of the hydrophilic/hydrophobic surfaces of cellulose I and cellulose II on the growth of CTF were determined. This is the first use of unmodified cellulose II as a template for the in situ growth of ultrathin CTF and provides important insights into dynamic CTF-cellulose interactions. This research provides a new cost-effective strategy for preparation of ultra-dispersed CTF based on large-scale cellulose templates.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 22
·13364-13373
·
IF 10.7
Lei Huang,Qian Wang,Zimo Wang,Xi Sun,Jiayu Guan,Jifu Zheng,Shenghai Li,Suobo Zhang
Balancing phosphoric acid (PA) uptake with the dimensional stability of PA-doped membranes is a major challenge in the field of high-temperature proton-exchange membranes. Crosslinking is a common method to solve this problem. However, the construction of conventional crosslinked membranes usually involves a two-step process in which linear polymers are first prepared, followed by the addition of crosslinkers during film formation to generate crosslinked networks. This further complicates the preparation process of crosslinked membranes. In this study, superacid-catalyzed Friedel–Crafts polyhydroxyalkylation was employed to fabricate knitted-network membranes with a high density of alkaline groups in a single step, significantly simplifying the preparation process of crosslinked membranes. Compared with commercial OPBI membrane, the knitted-network membranes exhibited significantly improved mechanical properties; moreover, PA retention was significantly improved, attributable to the formation of three-dimensional crosslinked networks and ultra-microporous structures within the membranes. Additionally, the PA-doped knitted-network membranes exhibited a good conductivity of 186 mS cm−1 at 200 °C and a high peak power density of 850 mW cm−2 at 200 °C without backpressure and humidification. This study is the first to report this in situ polymerization method in which the same precursor monomer is adopted in the subsequent polymerization process to form a crosslinked network. The proposed strategy exhibits significant application potential in the field of high-temperature proton-exchange membrane fuel cells.
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FUEL
·
2024
·
IF 6.7
Xiuzhu Zhang,Zongxue Yu,Junlei Tang,Jiaqiang Huang,Xunwang Tang,Bing Lin,Shuangshuang Xia
The improvement of ionic conductivity and alkali stability of anion exchange membranes(AEMs) has been the focus of research. The abundant functional groups on the surface of inorganic nanomaterials tend to form a rich hydrogen bonding network, which reduces the activation energy and improves the ionic conductivity. In this paper, the prepared HF-Ti 3 C 2 T x was used as a filler in a quaternized poly(aryl piperidinium) (QPAP) matrix to enhance the performance of the membrane electrode assembly of an anion exchange membrane water electrolyzers (AEMWE). With the addition of MXenes, the mechanical properties of the composite membrane improved significantly (from 12.13 MPa to 27.85 MPa). At 80 °C, the ionic conductivity of QPAP-HM-0.7 was as high as 159.4 mS cm −1 . The results showed that the functional groups on the surface of MXenes and the polymer matrix successfully constructed a hydrogen bonding network within the membrane, forming a hydrophilic and hydrophobic microphase separation structure. In addition, the composite membranes prepared by doping HF-Ti 3 C 2 T x obtained good alkali stability (conductivity retention of more than 85 % after 720 h immersion at 80 °C in 1 M NaOH) and dimensional stability, which proved that MXenes is an effective filler to improve the membrane properties.
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Journal of CO2 Utilization
·
2024
·
IF 7.2
Yan Yang,Xiaotian Liu,Jingfu Jia,Haojia Chen,Xing Mao,Chao Xiong,Hongbing Ji
With the intensification of the global greenhouse effect, the utilization and fixation of CO 2 has become one of the most important research fields in our world. However, there are still enormous challenges in achieving efficient fixation and conversion of carbon dioxide into high-value chemicals. Herein, the cycloaddition reaction strategy is adopted to achieve the fixation of supercritical carbon dioxide (SC-CO 2 ) and the high-value conversion of carbon resources to propylene carbonate (PC) by using propylene oxide (PO) as the reaction precursor. Under tetrabutylammonium bromide (TBAB) as a catalyst and water (H 2 O) as a green solvent, the reaction factors, such as reaction temperature, reaction pressure, catalyst amount, water concentration and molar ratio of reactants, is conducted through the high-throughput screening technology to explore the catalytic performance in a self-designed microchannel reactor. The results indicate that the yield of PC can reach 91.82 % (along with a high selectivity of 99.12 %) at a reaction temperature of 160 ℃, reaction pressure of 8 MPa, catalyst amount of 0.72 mol %, reactants molar ratio of 8, and the residence time of 482 s. Besides, the thermodynamic and kinetic for carbonate synthesis are studied to fully understand the reaction process, and the activation energy of is explored. This work is more efficient than most similar reported works, which provide valuable insights into the practical application of CO 2 in the supercritical state combined with microfluidics for synthesizing high-value monomers.
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AICHE JOURNAL
·
2024
·
IF 3.5
Yang Zhao,Qian Wang,Huifang Wu,Lirong Zheng,Zhexi Gao,Xuanlin Guo,Xingzhong Cao,Dianqing Li,Junting Feng
Reductive amination of biomass aldehydes is a vital process to synthesize chemical intermediates primary amine, but the selectivity is severely compromised by the self-condensation of highly reactive imine intermediates. Herein, we proposed a solution by manipulating the adsorption configuration of secondary imine via defect engineering. Specifically, a gradient reduction strategy was used to adjust the driving force of NiCo alloy crystallization, thus motivating the formation of metal vacancy clusters. The primary amine selectivity was raised from 70.9% to 95.1% with defect concentration increased from 36.1% to 42.5% on catalysts. In situ fourier transform infrared spectroscopy (FTIR) and density functional theory demonstrated metal vacancy clusters induced remarkable Ni Co electron transfer, which strengthened electronic coupling between secondary imine with catalyst, resulting in a flat configuration that was conducive to CN bond breakage to guarantee smooth conversion into primary amines. This catalyst exhibited potential real-life application prospects for its low cost, universality in reductive amination of various aldehydes, and long-life reusability.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jingyi Yang,Yongzhen Gao,Jie Fan,Jieqiong Wang,Tao Yang,Zezheng Bing,Meng Zhang,Zhongyi Liu
Tuning the metal-support interaction (MSI) between highly dispersed nanosized metal particles and the support plays a pivotal role in the activity and selectivity of polyaromatics selective hydrogenation. In this work, the supported bimetallic Ni-Ru/SiO 2 -SEA catalyst was prepared by a strong electrostatic adsorption (SEA) strategy, and applied for the selective hydrogenation of biphenyl (BP) to cyclohexylbenzene (CHB). Compared to the catalysts prepared by the conventional incipient wetness impregnation method and Ni/SiO 2 -SEA, the significant effects of MSI and hydrogen spillover on Ni-Ru/SiO 2 -SEA facilitated the highly exposed and uniformly dispersed electron-deficient Ni δ+ (0 < δ < 2) species, which could enhance adsorption and activation of the electron-withdrawing phenyl group and H 2 , thereby promoting the efficient and selective conversion of BP to CHB. At the conditions of 160 ℃ and 2 MPa H 2 pressure, BP conversion over Ni-Ru/SiO 2 -SEA reached nearly 100 % within 3 h, achieving a remarkable selectivity of 97.9 % towards CHB, along with a high turnover frequency of 2756.9 h −1 for the active metallic Ni sites. Importantly, according to the kinetic simulations, the hydrogenation rate constant of Ni-Ru/SiO 2 -SEA was the highest (2.76 × 10 -2 mol·g −1 ·h −1 ) among the employed catalysts. Moreover, after six consecutive cycles, no obvious decline in hydrogenation efficiency was observed, confirming the remarkable activity and stability of Ni-Ru/SiO 2 -SEA. Furthermore, the activation of BP and desorption of CHB pathway on the Ni δ+ species were elaborated through temperature-programmed desorption characterization, highlighting the prominent contribution of MSI in enhancing the selective hydrogenation of polyaromatics.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 5
·1989-1998
·
IF 3.5
Yanshu Liu,Guanyun Zhang,Dexin Wang,Guanjie Chen,Fangfang Gao,Chen-Ho Tung,Yifeng Wang
A cryptand-like Ti-coordination compound, namely Ti12Cs, comprising two Ti6-salicylate cages and hosting two Cs+ ions, was synthesized by the solvothermal method. It exhibits strong visible-light absorption with an absorption band edge of 652 nm, attributed to the electron transition from salicylate ligands to Ti ions. Electrochemical impedance, visible-light transient photocurrent response, and photoluminescence spectra confirm that Ti12Cs has excellent visible-light response and charge-separation properties. Ti12Cs can be used as a heterogeneous and recyclable photocatalyst for CO2/epoxide cycloaddition, with high utilization efficiency of visible-light under mild conditions. The mechanism investigation points to a synergistic effect of photocatalysis and Lewis acid catalysis.
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高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Yali Yang,Jia Chen,Xiaojing Liang,Bei Liu,Kaijun Quan,Xiuhui Liu,Hongdeng Qiu
In this paper, three imidazole- and C18- bifunctional silica stationary phases (Sil-Im-C18) were prepared by adjusting introduction interval of octadecyltrichlorosilane (ODS) and 3-imidazol-1-ylpropyl(trimethoxy)silane (TMPImS), which can be used for reversed-phase liquid chromatography (RPLC) and ion exchange chromatography (IEC) with adjustable performance. The successful preparation of Sil-Im-C18 were confirmed by the characterizations of elemental analysis, infrared spectroscopy (FTIR) and contact angle (CA). Chromatographic performance of Sil-Im-C18 were evaluated by the separation of Tanaka test mixture, alkylbenzenes, linear PAHs and a set of analytes with different properties (uracil, phenol, 1,2-dinitrobenzene and naphthalene), and compared with commonly used C18 column. It was found that the chromatographic performance of Sil-Im-C18 changed significantly with the difference in bonding amount of imidazole and C18. Sil-Im-C18 demonstrated the excellent separation performance towards polycyclic aromatic hydrocarbons (PAHs), phenylesters, phenylamines , phenols and inorganic anions, and notably, nucleobases and nucleosides can be separated using pure water as mobile phases . The van Deemter plot showed that the column efficiency of Sil-Im-C18-3 was 64,933 plate· m − 1 for naphthalene, indicated that Sil-Im-C18 was reasonably chromatographic columns. The RSD values of retention time were 0.22 %-0.61 % for 10 needles alkylbenzenes injected continuously at 50 °C to investigate thermal stability and repeatability, all the fluctuations of k of naphthalene were less than 2.3 % for Sil-Im-C18-1 during flushing 24 h with the mobile phase at different pH values (pH = 3 and 8), the retention time of alkylbenzenes were almost same for Sil-Im-C18-1 at different time, the RSD values of retention time of alkylbenzenes were 0.45 %-2.28 % for two batches Sil-Im-C18-1, revealing the excellent repeatability, thermal stability, durability and reproducibility of Sil-Im-C18, and implying a commercial prospect.
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Polymers
·
2024
·Vol. 16
·期 15
·2208
·
IF 4.7
Kun Cai,Jinzhu Yu,Wenjun Tan,Cong Gao,Zili Zhao,Suxin Yuan,Jinghui Cheng,Yajie Yang,Ye Yuan
Nafion membranes are widely used as proton exchange membranes, but their proton conductivity deteriorates in high-temperature environments due to the loss of water molecules. To address this challenge, we propose the utilization of porous aromatic frameworks (PAFs) as a potential solution. PAFs exhibit remarkable characteristics, such as a high specific surface area and porosity, and their porous channels can be post-synthesized. Here, a novel approach was employed to synthesize a PAF material, designated as PAF-45D, which exhibits a specific surface area of 1571.9 m2·g−1and possesses the added benefits of facile synthesis and a low cost. Subsequently, sulfonation treatment was applied to PAF-45D in order to introduce sulfonic acid groups into its pores, resulting in the formation of PAF-45DS. The successful incorporation of sulfonic groups was confirmed through TG, IR, and EDS analyses. Furthermore, a novel Nafion composite membrane was prepared by incorporating PAF-45DS. The Nyquist plot of the composite membranes demonstrates that the sulfonated PAF-45DS material can enhance the proton conductivity of Nafion membranes at high temperatures. Specifically, under identical film formation conditions, doping with a 4% mass fraction of PAF-45DS, the conductivity of the Nafion composite membrane increased remarkably from 2.25 × 10−3S·cm−1to 5.67 × 10−3S·cm−1, nearly 2.5 times higher. Such promising and cost-effective materials could be envisioned for application in the field of Nafion composite membranes.
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