ACS Applied Energy Materials
·
2020
·
IF 4.473
Xiuwei Sun,Shumei Liu,Shan Zhang,Tianyi Dang,Hongrui Tian,Ying Lu,Shuxia Liu
Almost all proton-conducting materials display poor conductivity at subzero temperatures, which significantly limits their application in cold regions. Thus, effective strategies to achieve high proton conductivity in a wide range from subzero to medium temperatures (−40 to 85 °C) need to be developed. Herein, we prepared proton-conductive materials by encapsulating the acid–base adduct based on Keggin-type H3PW12O40 (HPW) and aminoethanesulfonic acid (C2H7O3NS, HSN) in the linear channels of SBA-15 (named HPW-HSN@SBA-15). The result is the same as we expected: HPW-HSN@SBA-15 exhibits high proton conductivity over a wide temperature range (−40 to 85 °C). The proton conductivity of 75 wt % HPW-HSN@SBA-15 (3HPW-HSN@SBA-15) reaches 0.16 S cm–1 at 85 °C, 97% relative humidity (RH), and 6.8 × 10–5 S cm–1 at −40 °C. The excellent proton conductivity at subzero temperature of HPW-HSN@SBA-15 is mainly attributed to the ultrafast proton transfer with low energy barrier between proton donor (acid group) and proton acceptor (base group) in acid–base adduct without the attendance of water. Furthermore, the proton conductivity cycle test of 3HPW-HSN@SBA-15 demonstrates its good durability and stability.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Xiuwei Sun,Xue Bai,Qian Wang,Ying Lu,Shuxia Liu
Most reported proton-conducting materials use water molecules as media for proton transport, but their low operating temperatures (below the boiling point of water) and humidity-dependent conductivity limit their extensive applications. This motivated researchers to explore high-temperature proton-conducting materials employing nonaqueous media. The acid–base adduct HPW-SA formed by Keggin-type phosphotungstic acid (H3PW12O40, abbreviated as HPW) and sulfamic acid (SA) shows high proton conductivity in the high-temperature region (160–190 °C), owing to its proton mobility remarkably enhanced by its solid–liquid transition. Inspired by this, we encapsulated the HPW-SA adduct into the cages of MIL-101 by the postsynthetic method to prepare the composite HPW-SA@MIL-101, aiming at taking full advantage of the proton conduction feature of the HPW-SA adduct while avoiding the problems of flowing away and corrosion caused by the independent use of HPW-SA adduct. As expected, HPW-SA@MIL-101 exhibits high proton conductivity (0.85 × 10–3–1.1 × 10–3 S cm–1) in the range of 160–190 °C. Its proton transfer activation energy (Ea) is 0.58 eV in the range of 160–190 °C, which indicates that proton migration is dominated by the diffusion effect following a vehicle mechanism. In addition, the proton conductivity of HPW-SA@MIL-101 did not decrease after six cycles of heating and cooling tests, showing good repeatability and stability.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 9
·2369
·
IF 5.076
Bao Wang,Lihua Kang,Mingyuan Zhu
A hierarchical porous carbon material (HPC) with an ultra-high specific surface area was synthesized with sisal fiber (SF) as a precursor, and then H3PW12O40·24H2O (HPW) was immobilized on the support of SF-HPC by a simple impregnation method. A series characterization technology approved that the obtained SF-HPC had a high surface area of 3152.46 m2g−1with micropores and macropores. HPW was well-dispersed on the surface of the SF-HPC support, which reduced the loading of HPW to as low as 5%. HPW/SF-HPW showed excellent catalytic performance for oxidative desulfurization, and the desulfurization rate reached almost 100% under the optimal reaction conditions. The desulfurization rate of HPW/SF-HPW could be maintained at above 94% after four recycles.Keywords:oxidative desulfurization;hierarchical porous carbon;HPW loading;dispersion
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
Processes
·
2022
·Vol. 10
·期 2
·402
·
IF 3.352
Ziyang Zheng,Qian Wu,Shengyang Zhong
In this work, polyacrylamide (PAM) was first used in the loading of heteropoly acids, and then the HPM/PAM-n catalyst was synthesized by simple reaction. The FTIR and SEM measurements showed that the HPM/PAM-n (n = 10,000, 20,000, 30,000) was successfully synthesized. In addition, the HPM/PAM-n effect on desulfurization was measured, which showed the optimal desulfurization efficiency. The optimal process condition for HPM/PAM-10000 desulfurization was optimized by a single-factor experiment. The optimal condition was as follows: The temperature was 60 °C, the amount of the catalyst was 0.2 g, the oxygen to sulfur ratio was 16, and the reaction time is 100 min. The catalyst was suitable for recycled use, and the desulfurization efficiency was high after 10 times. In the end, the oxidative desulfurization mechanism was put forward.Keywords:PAM;desulfurization;heteropoly acid;recycle use
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2021
·Vol. 100
·期 7
·1558-1568
·
IF 2.007
Jian Chen,Mengjing Zhu,Fuwei Xiang,Junfeng Li,Hongjun Yang,Zhipeng Mao,Ganggang Chang,Shaoping Li
(2-methyl-6-ethylphenyl)-1-methoxypropyl-2-imine (MEMI) is an important intermediate for the synthesis of commercial pesticide S-metolachlor. However, the research on heterogeneously catalytic kinetics of MEMI, and further the catalytic distillation simulation aiming at continuous operation, have never been reported. Herein, the catalytic kinetics for the synthesis of MEMI by HPW/Al-MCM-41 have been systematically investigated, and further fitted by using a pseudo-homogeneous kinetic model, based on which, the reaction equilibrium constant, activation energy, and rate constant are obtained. Furthermore, simulation of the continuous process of MEMI synthesis was carried out using the software Aspen Plus V10. Sensitivity analysis of operating parameters such as feed stage, distillation rate, number of reactive theoretical stages, and the best operating conditions were also obtained. An excellent product purity (>98.9%) of MEMI could be achieved when operated at the optimum conditions. Compared with the batch method, catalytic distillation provided continuous synthesis of MEMI, and the reaction was more thorough, achieving process integration and optimization. Our results provide substantial theoretical and empirical supports for the industrial synthesis of MEMI.
研究领域:
化学工程
·
催化反应工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Mingzu Liu,Xiuxiu Zhao,Zefeng Ma,Bing Yuan,Fengli Yu,Congxia Xie,Shitao Yu
As a naturally rigid polycyclic biomass platform compound without oxygen, α-pinene has always been expected to develop high-energy–density fuel with both good combustion performance and cryogenic properties by increasing carbon number in a high atom economical way. The present work has explored the screening of alkylation blocks for α-pinene over H 3 PW 12 O 40 (HPW). Here, a novel pinene-based blended fuel was prepared through cross-alkylation of α-pinene with mixed isobutane/isobutene, the common low-cost feedstock of alkylated gasoline. The reaction conditions including feed composition, reaction time, catalyst dosage, and reaction temperature were optimized. The mechanism of the hybrid alkylation process was further computationally speculated and experimentally verified. Produced liquid hydrocarbon products after hydrogenation and vacuum distillation possessed higher net heat of combustion and flash point than those of pinane, and lower freezing point and viscosity than those of dimers fuel from pinene. These favorable performances indicate that alkylated pinanes have promising potential as high-energy aviation fuel.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Tingting Sun,Xinwei Zhang,Yisheng Hu,Lei Xu,Yahui Zhao
The UiO-66-FP/HPW/TiO 2 heterojunction photocatalytic material is fabricated by one-pot solvothermal method. The crystal structure, elemental composition, morphology, and optical properties of as-prepared catalysts are well-characterized. Subsequently, the synthesized materials’ catalytic activity is evaluated by degrading rhodamine B (RhB) and ofloxacin (OFX) under visible-light illumination. It turns out that the 10 wt% UiO-66-FP/HPW/TiO 2 sample possesses the best efficiency, with 98.6% RhB and 97.2% OFX removed under identical condition, which is 4.68 and 4.14 times than that of HPW/TiO 2 , respectively. The superior efficiency can be ascribed to the construction of UiO-66-FP/HPW/TiO 2 heterostructure, better adsorption capacity of organic contaminants, enhanced visible light response, and lower recombination rate of e − -h + pairs. The quenching effect of distinct scavengers indicates that •OH is an additional significant contributor to the ternary photodegradation system besides •O 2 – and h VB + species. This constitutes another reason for the superior photocatalytic activity of UiO-66-FP/HPW/TiO 2 relative to HPW/TiO 2 . The photo-degradation efficiency of 10 wt% UiO-66-FP/HPW/TiO 2 composite is reduced by 4.68% after running five cycles. Overall, this work presents one type of efficient and reusable TiO 2 -based photocatalysts driven by visible light.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2026
·
IF 3.6
Lai Wei,Zhendong Yu,Haofeng Wu,Xiaoxiao Xing,Yiru Zou,Limin Song,Peiwen Wu,Minmeng Tang,Xiaoxiao Yu,Wenshuai Zhu
The catalytic oxidation of aromatic sulfides under mild, ambient conditions facilitates the high-value utilization of diesel fuel, free from external heating sources. Herein, a high-performance confined catalyst through a simple one-pot method is developed, denoted as HPW@ZIF-8. The phosphotungstic acid is encapsulated and confined within the pores of the ZIF-8 framework, achieving ambient temperature catalytic oxidation of aromatic sulfides to high-value sulfones. The induced charge shift in the confined catalysis is observed, as the weak interaction force between the phosphorus-tungsten structure and Zn center, strengthening the catalytic oxidation performance. Under unheated conditions, the hydrogen peroxide utilization rate and activity of the catalyst at ambient temperature are both greater than 97.0%. In addition, the confined catalysts exhibit good cycling performance after 10 cycles, attributed to the highly matched host and guest, with only 0.2% HPW loss. Above all, this work offers new insights for the green, low-energy consumption, and high-value utilization of diesel fuel. Graphical Constructing confined catalytic materials by encapsulating active centers in the cavities of ZIF-8 metal-organic frameworks. This strategy enables the efficient catalytic oxidation of sulfur-containing compounds in diesel to high-value sulfone products at ambient temperatures. This produces ultra-low diesel with a sulfur content of less than 10 mg/L.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sensors
·
2026
·Vol. 11
·期 8
·7558-7571
·
IF 10.9
Cao Chen-Yang,Cheng Chen,Yue Li-Juan,Xie Ke-Feng,Dong Hua-Dong,Yang Xuan-Yu,Zhang Yong-Hui
Rational design of interfacial electronic structures and defect sites is pivotal for advancing chemiresistive gas sensing, yet achieving synergistic modulation remains a formidable challenge. Herein, we report a ternary Pd–HPW–ZnO heterostructure constructed via the integration of phosphotungstic acid (HPW) clusters and Pd nanoparticles onto porous ZnO nanosheets. This unique architecture establishes a robust electronic coupling network, where HPW acts as an electron sink, inducing electron depletion in both ZnO and Pd species to form electron-deficient Pd sites. This electronic modulation, corroborated by XPS and DFT calculations, significantly optimizes the Pd d-band center and enhances the surface Lewis acidity. Furthermore, the synergistic interaction triggers a substantial enrichment of oxygen vacancies and facilitates the spillover of active oxygen species. Consequently, the optimized sensor exhibits an extraordinary response of 2016.70 to 50 ppm triethylamine (TEA) at a low operating temperature of 110 ° C, surpassing pristine ZnO by nearly 60-fold. The sensor also demonstrates ultrafast response/recovery kinetics (16/150 s), excellent selectivity against interfering volatiles, and robust long-term stability. This work provides a paradigm for boosting sensing performance through precise interfacial electronic regulation and defect engineering in multicomponent heterostructures.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
POLYMER
·
2023
·
IF 4.6
Peng Wei,Dong Huang,Chen Luo,Yang Sui,Xi Li,Qingkun Liu,Bensheng Zhu,Chuanbo Cong,Qiong Zhou,Xiaoyu Meng
Due to its uncomplicated manufacturing procedure for large-scale industrialization and adaptable conductivity, the competitive proton exchange membrane (PEM) matrix employed is sulfonated poly (ether ether ketone). However, the conflict between the strong proton conductivity and high stability of SPEEK-based PEM constantly upsets the equilibrium; the primary chain of SPEEK will conduct more protons if additional sulfonic acid is introduced, but it also causes a high swelling ratio and lowers stability. To tackle this challenging issue, we coupled the high intrinsic proton conductivity of phosphotungstic acid (HPW) and the excellent stability of polyimide (PI) nanofibers in a single PEM. In particular, sandwich-structure hybrid membranes (PI/SPEEK + HPW) were created to reduce HPW loss under operational conditions, further improving stability. Consequently, the swelling ratio and conductivity of the premium sandwich-structure PI/SPEEK + HPW-20 were 29% and 223.4 mS cm −1 under 60 °C and 100% RH, their respective values were 8% larger than those of SPEEK. Its proton conductivity reached 170.9 mS cm −1 during 13 days of exposure under 60 °C and 100% RH, which would be 30% better than that of SPEEK over the same treatment. Protons in these membranes were transported through Grotthus and vehicle mechanism, and the establishment of an acid-rich layer at the surface among PI nanofiber with HPW/SPEEK, which was confirmed by FTIR, XPS , and TEM , is responsible for these superior performances. From our point of view, our findings might encourage more studies into the creation of high-performance PEM.
研究领域:
材料科学
·
高分子化学
·
能源材料
·
电化学
·
膜科学与技术
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS
·
2021
·Vol. 54
·期 2
·71-80
·
IF 1.462
Yufei Yang,Yadong Zhang
In this work, a HPW/ZSM-5 catalyst was prepared by impregnating phosphotungstic acid (HPW) with carrier ZSM-5 zeolite and characterized by XRD, SEM, N 2 adsorption/desorption isotherm, NH 3 -TPD, and FT-IR techniques. The catalytic performance of HPW/ZSM-5 was investigated by using the decomposition reaction of cyclohexylbenzene-1-hydroperoxide (CHBHP) to phenol and cyclohexanone. The conversion rate of CHBHP was up to 97.28%. In addition, the reusability test exhibited that the high durability HPW/ZSM-5 as the conversion rate of CHBHP only decreased by 3.11% after five runs. The kinetic study of the decomposition reaction indicated it was a primary reaction. The apparent activation energy of the decomposition reaction was 102.39 kJ·mol –1 in the temperature range of 45–60℃. All results indicate that the HPW/ZSM-5 catalyst has good performance and promising applications in acid catalyzed organic chemistry.
研究领域:
催化化学
·
有机化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Zhaoyang Qi,Huaifang Li,Jie Chen,Changshen Ye,Ting Qiu
The carboxyl functionalized ionic liquid ([mim(CH 2 ) 3 COOH]Cl) was prepared as a linker to combine phosphotungstic acid (HPW) and Zr(IV) ion. The obtained [mim(CH 2 ) 3 COO] 3 PW-Zr composite acted as a heterogeneous catalyst for removing DBT from liquid fuel with H 2 O 2 as an oxidant. As a result, [mim(CH 2 ) 3 COO] 3 PW-Zr possessed high catalytic activity in extractive and catalytic oxidative desulfurization (ECODS). Moreover, the [mim(CH 2 ) 3 COO] 3 PW-Zr was further exploited to grow on the surface of PEI/silica gel. And the fabricated large-grained Zr-PWIL@PEI/silica gel was used in the continuous ECODS process, and the removal of DBT could still reach more than 95% after running continuously for 16 h. More importantly, the synergistic catalytic mechanism between HPW and Zr(IV) in the ECODS process has been investigated in detail by experiments and DFT calculations. As a result, a plausible mechanism has been proposed and verified, which contains two parts: the Lewis acidic center activating H 2 O 2 to form superoxide ion radicals ( OOH), and the OOH oxidizing HPW to peroxotungstate (W(O 2 ) n ), which has a high oxidizability and stability. Thus, the effective combination of Zr(IV) and HPW active sites is a very effective strategy to promote desulfurization efficiency and utilization efficiency of H 2 O 2 . Besides, we also found the distance between the corresponding active sites of catalysts plays an essential role in ECODS reaction as it strongly influences the synergistic effect between different active sites.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）