DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 8
·3666-3674
·
IF 3.5
Amir Said,Guanjie Chen,Guanyun Zhang,Dexin Wang,Yanshu Liu,Fangfang Gao,Guo Wang,Chen-Ho Tung,Yifeng Wang
Titanium-oxide clusters (TOCs) are well-defined molecular models for TiO2 materials and provide the opportunity to study the structure–activity relationships of TiO2. Here, we report a new Pb-doped TOC, Ti12Pb2, which resembles a two-layer decker of the {TiTi6} structural units of rutile TiO2 with two Ti4+ ions replaced by two Pb2+ ions. Its electronic structure, photoresponse, and photocatalytic performances were investigated and compared with those of the Ti14 cluster, which is isostructural to Ti12Pb2. Our results indicate that Pb2+ does not affect the electronic structure, but it greatly enhances the photocatalytic activity by improving the charge-separation and interfacial charge-transfer properties of the TOC. The successful synthesis of Ti12Pb2 highlights the roles of closed-shell heterometal ions in the construction of new TOCs. Our mechanism may be an inspiration for understanding the structure–activity relationships of closed-shell heterometal-doped TiO2.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Timur Meng,Xianhao Liu,Yuyue Peng,Hongliang Lei,Zhiyi Li,Saowaluk Chaleawlert-umpon,Yutong Dai,Kaige Zhao,Lina Li
The precise control of pore structures in porous organic polymer (POP) materials is of paramount importance in addressing a wide range of challenges associated with gas separation processes. In this study, we present a novel approach to optimize the gas separation performance of POPs through the introduction of fluorine groups and figure out an important factor of reaction decision that whether the AlCl3-catalyzed polymerization is Scholl reaction or Friedel–Crafts alkylation. In the chloroform system, the steric hindrance of function groups could make direct coupling between the benzene rings difficult, which would lead to part solvent knitting (Friedel–Crafts alkylation) instead. The fluorinated polymers show enhanced surface area and pore size characteristics. Notably, the fluorinated polymers exhibited significantly improved adsorption and separation performance for SF6, as evidenced by an ideal adsorbed solution theory selectivity (SF6/N2, v: v = 50:50, 273 K) increase of 75.0, 668.8, and 502.8% compared to the nonfluorinated POPs. These findings highlight the potential of fluorination as a strategy for tailoring the properties of POP materials for advanced gas separation applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Wenli Ma,Lin Tian,Qingqing Zhu,Shuhuan Zhang,Fanghui Wang,Hong Zhu
To prepare anion exchange membranes with high water electrolysis and single fuel cell performance, an inorganic–organic composite (IOC) strategy with click cross-linked membranes coated with different contents of hydrophilic polar nanozirconia is proposed to fabricate composite membranes (CM) PBP-SH-Zrx. The performance test results showed that the CM PBP-SH-Zr4 not only has good through-plane ionic conductivity (167.7 mS cm–1, 80 °C), but also exhibits satisfactory dimensional stability (SR 16.5%, WU 206.4%, 80 °C), especially demonstrating excellent alkaline stability with only 16% degradation (2 M NaOH for 2200 h). In water electrolysis, the “microgap” between the membrane and catalyst layer (solid–solid interface) is alleviated, and the membrane electrode assembly (MEA) interfacial compatibility (liquid–solid–solid interface) is enhanced. The CM PBP-SH-Zr4 showed the lowest charge transfer resistance (Rct, 0.037 Ω cm2) and a high current density of 2.5 A cm–2 at 2.2 V, while the voltage drop was 0.361 mV h–1 after 360 h of endurance (six start–stop cycles) at 60 °C and 500 mA cm–2, proving a good water electrolysis durability. Moreover, an acceptable peak power density of 0.464 W cm–2 at 80 °C is achieved in a H2/O2 fuel cell with a PBP-SH-Zr4-AEM. Therefore, the IOC strategy can enhance the membrane’s comprehensive performance and interface compatibility of MEA and may promote the development of anion exchange membranes (AEMs) for water electrolysis and fuel cells.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meifang Cao,Yuqiao Ma,Tao Ruan,Lifeng Li,Bo Chen,Xueqing Qiu,Di Fan,Xinping Ouyang
The cleavage of C-O bonds in lignin depolymerization was made great progress, but the cleavage of C-C bonds still face challenges. An atomically dispersed Pt loading of 3.30 wt% catalyst, Pt/Nb 2 WO 8 , was prepared by the pyrolysis of ammonium niobate oxalate and sodium tungstate dihydrate with ammonium carbonate as the template. It is found that the decomposition of ammonium carbonate and the doping of W species promoted the orderly growth of niobium tungsten oxide crystals with oxygen vacancy and the formation of a regular porous structure, which was conducive to the dispersion of Pt particles. Pt/Nb 2 WO 8 efficiently cleaved β-O-4, β-1, α-1 and 5–5 bonds. The yield of aromatic monomers for lignin depolymerization reached as high as 49.08% over Pt/Nb 2 WO 8 . Experiments combined with density functional theory calculations revealed that the excellent activity of the Pt/Nb 2 WO 8 catalyst was attributed to the cooperation of atomically dispersed Pt sites and support near the interface. The atomically dispersed Pt species enhanced the dissociation of H 2 , and the Nb 2 WO 8 support with abundant B acid sites provided by W doping and oxygen vacancies activated C-O and C-C bonds of lignin in the reaction. The homogeneous cleavage of C-C bonds dominated the deconstruction of β-1, α-1 and 5–5 bonds. This methodology opens up a facile strategy for the design of atomically dispersed Pt/Nb 2 WO 8 catalyst with higher Pt loading and excellent catalytic activity to the cleavage of both C-O and C-C bonds in lignin.
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2024
·
IF 4.6
Tianlan Yan,Yingshuai Jia,Kaige Hou,Zhuxin Gui,Wenbiao Zhang,Ke Du,Di Pan,He Li,Yanghao Shi,Lu Qi,Qingsheng Gao,Yahong Zhang,Yi Tang
Hydrodesulfurization (HDS) is a commonly used route for producing clean fuels in modern refinery. Herein, ammonium/amine-intercalated MoS 2 catalysts with various content of 1T phase and S vacancies have been successfully synthesized. Along with the increment of 1T phase and S vacancies of MoS 2 , the initial reaction rate of the HDS of dibenzothiophene (DBT) can be improved from 0.09 to 0.55 μmol·g cat −1 ·s −1 , accounting for a remarkable activity compared to the-state-of-the-art catalysts. In a combinatory study via the activity evaluation and catalysts characterization, we found that the intercalation species of MoS 2 played a key role in generating more 1T phase and S vacancies through the ‘intercalation-deintercalation’ processes, and the hydrogenation and desulfurization of HDS can be significantly promoted by 1T phase and S vacancies on MoS 2 , respectively. This study provides a practically meaningful guidance for developing more advanced HDS catalysts by the intercalated MoS 2 -derived materials with an in-depth understanding of structure-function relationships.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Hongjing Li,Min Liu,Bin Hu,Xu Hu,Meizi He,Junhao Xin,Chengyuan Niu,Yingda Huang,Nanwen Li,Zushun Xu,Quanyuan Zhang
Porous separators are essential for alkaline electrochemical energy technologies, such as alkaline water electrolyzers (AWEs). These separators are promising alternatives to dense membranes because they offer the potential for low cost and high ionic conductivity. However, two significant challenges in developing efficient and durable alkaline energy systems are the suppression of hydroxide ions-induced degradation and the reduction of gas permeation in porous separators. Compared to hydrophobic polysulfone (PSF), KOH-doped poly (oxindole biphenylene) (POBP) is a highly stable ion-solvating polymer that can conduct both potassium and hydroxide ions. Building upon this, a series of porous separators based on POBP polymer with different zirconia loads were designed using NIPS to investigate the chemical stability and water electrolysis performance where the Z60 separator exhibits remarkable characteristics, including low area resistance (0.227 Ω cm 2 ), high bubble point pressure (0.813 MPa), low H 2 permeability (0.5 L min −1 ·cm −2 ) and exceptional 5040 h of ex-situ durability in 6 M KOH at 80 °C. Furthermore, the Z60 diaphragm showed a higher breaking time and lower weight loss after 261 h at 80 °C in the Fenton reagent, with the remaining mass being Z60 was 38 %. Notably, the Z60 diaphragm, when equipped with Ni–Al catalysts, achieved a current density of 0.5 A/cm 2 at 1.7 V, which surpasses that of Zirfon (0.5 A/cm 2 at 1.8 V). More importantly, when using Ni foam catalysts, the Z60 diaphragm demonstrated stable operation under 0.125 and 0.5 A/cm 2 current densities at 80 °C for more than 900 h and 1200 h, significantly improving the durability of the porous separators. The results of this study showed that the blending of POBP can lead to the development of highly chemically stable porous diaphragms, thereby opening up a new avenue for advanced AWEs.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Lei Huang,Jiayu Guan,Xi Sun,Guorui Qin,Jifu Zheng,Shenghai Li,Suobo Zhang
The development of high-temperature proton-exchange membranes (HT-PEMs) with high phosphoric acid uptake (PU) and adequate mechanical strength presents a significant challenge. Researchers widely recognize crosslinking as an effective approach to address the conflict between mechanical strength and PU in phosphoric acid-doped membranes. Generally, crosslinked networks are constructed in an alkaline environment, limiting the scope of crosslinked membranes. Based on the Friedel–Crafts reaction, which occurs between carbocation ions and electron-rich skeletons or groups under acidic conditions, this study utilized a novel bifunctional 1,3-adamantanediol as a stereocrosslinker to construct a crosslinked network. The unique three-dimensional structure of the crosslinker resulted in a large free volume within the polymer networks during crosslinking, facilitating the formation of a continuous proton transfer network. Notably, compared with linear polybenzimidazole polymer (PBI), the crosslinked membranes exhibited significantly higher PA retention due to the presence of ultra-microporous structures. Additionally, the number of imidazole units remained unchanged due to the crosslinking site on the aromatic ring. As anticipated, the PA-doped crosslinked membranes exhibited a high conductivity of 167 mS cm −1 and an excellent peak power density of 865 mW cm −2 at 200 °C. Based on the generality of the crosslinking reaction with stereocrosslinkers and the expansion of the range of reaction media, this study proves a new insight into the fabrication of the high-performance HT-PEMs.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Yu Chen,Zongxue Yu,Junlei Tang,Xiuzhu Zhang,Shijie Guo,Xunwang Tang,Zhiquan Chen,Yingqing Zhan
As one of the core components of anion exchange membrane water electrolyser (AEMWE), the performance of anion exchange membrane (AEM) has a direct impact on the application effect of the water electrolyzer. Chemical cross-linking method is an effective way to solve the problem of balancing membrane dimensional stability and ionic conductivity and improve mechanical properties. However, the crosslinked network brings hindrance to the ionic transport rate and causes the loss of ionic conductivity, having a direct impact on the application effect of water electrolysis. In this paper, a series of Poly(biphenyl-co-m-triphenyl-piperidine) (PBMP) based on composite AEMs are prepared by functionalized modification of MXene with high electrical conductivity as an inorganic cross-linking agent, and the electrical conductivity of MXene overcomes the hindrance of cross-linking on ion transport. Inorganic crosslinkers are classified into hexane hydrocarbon crosslinkers (6-NH 2 -Alk-Ti 3 C 2 T x ) and ethane hydrocarbon crosslinkers (2- NH 2 -Alk-Ti 3 C 2 T x ). The AEMs prepared with 2-NH 2 -Alk-Ti 3 C 2 T x crosslinker exhibit higher ionic conductivity (112.0 mS cm −1 ) due to a sharper microphase separation morphology. The presence of a crosslinked network within the membrane reduces the swelling ratio of the membrane (80 °C, 1.2 %) and improves the mechanical properties (from 29.2 MPa to 55.3 MPa). In addition, the AEMWE prepared by PBMP-0.46-2-NH 2 -Alk-Ti 3 C 2 T x (PBMP-0.46–2M) membrane reaches 760 mA cm −2 at 2.0 V, 70 °C in 1 M KOH solution. Therefore, it is feasible to realize AEMs prepared with functionalized MXene as crosslinker and filler for application in electrolysis cells.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Fei Gao,Qing Lu,Shougui Wang,Guanghui Chen,Pan Zhang,Yingxuan Wen,Fangfang Zhang,Jipeng Dong
Developing effective metal- and halogen-free heterogeneous catalysts for the CO 2 cycloaddition remains a challenge. In this study, novel imidazole-based hyper-crosslinked polymers (HCP-BZ, HCP-BP and HCP-TBZ) with abundant N sites were constructed via a one-pot polymerization, and employed as heterogeneous catalysts for the CO 2 cycloaddition reaction. The special skeletal pore structure with abundant hierarchical pore structures and uniformly distributed active sites were demonstrated by various characterization technologies. The optimal HCP-TBZ(16:1) exhibits a good CO 2 selective adsorption performance with a CO 2 adsorption capacity of 2.23 mmol/g and CO 2 /N 2 adsorption selectivity of 41 at 273 K and 0.1 MPa. Additionally, the resulting catalyst HCP-TBZ(16:1) achieves an excellent catalytic performance with 96 % yield and 99 % selectivity without metal, halogen, cocatalyst and solvent additions (120 °C, 1.0 MPa CO 2 , 5 h). Moreover, the HCP-TBZ(16:1) also exhibits a satisfactory catalytic activity under the mild conditions (70 °C, 1.0 MPa CO 2 ), and can effectively catalyze the cyclic carbonate preparation from the dilute CO 2 (15 %CO 2 /85 %N 2 ). The comparable catalytic activity and the determined structural stability, reusability and universality make the prepared imidazole-based HCPs a potential heterogeneous catalyst candidate for the CO 2 cycloaddition. This study will provide some guidance for developing metal-free and halogen-free CO 2 adsorption and conversion platforms.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 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）