ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yonghou Xiao,Qiang Guo,Shuohan Yang,Qidong Zhao,Gaohong He
The cuprous-ion-based zeolites constructed by introducing Cu(I) adsorption active sites into zeolite Linde Type A have proved to be efficient in carbon monoxide (CO) adsorption with high selectivity and capacity. However, how to directly fabricate zeolite 4A containing copper species and effectively overcome cuprous ion aggregation during the preparation process is still a challenge. Here, we propose an efficient fabrication method to synthesize highly dispersed Cu(I)-modified octahedral zeolite 4A adsorbents using a molecular complex formed by a hydrogel with a silicon/aluminum molar ratio of 1:1, copper ions, and tetramethylammonium hydroxide (TMAOH) as the template. Zeolite 4A containing copper ions was directly obtained by incorporating the precursor of cuprous ions into the confined space between zeolite 4A channel walls and TMAOH. The target zeolite Cu(I)/4A adsorbent with highly dispersed Cu(I) was constructed after introducing VCl3 as the reducing agent via the solid-state dispersion method during the process of removing the template. In comparison with pristine zeolite 4A, a bimodal microporous pore size distribution was observed in as-synthesized Cu(I)/4A. Cu(I)/4A exhibited an enhanced static (1.15 mmol/g) and dynamic (0.0016 mmol g−1) CO adsorption capacity, respectively, at 25 °C and 1 bar. Moreover, Cu(I)/4A displayed a lower H2 adsorption capacity under identical conditions. Through calculation using the ideal adsorption solution theoretical (IAST) equation, the CO selectivity from the CO/H2 mixture on Cu(I)/4A attained ca. 16.95. Therefore, Cu(I)/4A with highly dispersed Cu(I) was successfully fabricated, and its excellent CO adsorption selectivity and capacity enable it to be potentially applied for the actual deep separation of CO/H2.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Shuyan Lin,Yongxiang Wang,Xinyu Jing,Haonan Shen,Yide Hao,Zongyu Zhang,Jiangshan Gao,Yan He
The agglomeration phenomenon of metals in transition metal-based carbon catalysts has been one of the major reasons hindering their replacement of commercial Pt/C. Its self-aggregation phenomenon greatly limits the number of active sites and reactivity, which affects the catalytic performance. To overcome this issue, this work prepared a high N-doped carbon structure catalyst coated with high-dispersion FeCo/Fe 3 C nanoparticles. This was achieved by utilizing the advantages of the Prussian blue analogs (PBA) metal framework structure to suppress the self-aggregation of metals, thereby achieving high dispersion. Additionally, the introduction of melamine compensated for the nitrogen loss caused by the carbonization of PBA, thus increasing the nitrogen doping content. The experimental results show that when the calcination temperature is 850 °C and the mass ratio of melamine to FeCo PBA is 5, the half-wave potential (E 1/2 ) of the FeCo@NC catalyst prepared can reach 0.857 V, and the current intensity of FeCo@NC catalyst can maintain 97.12 % during 40,000 s stability test, which is much higher than that of commercial Pt/C. Moreover, the prepared FeCoNC@-850-5 and commercial Pt/C catalysts were used as cathode catalysts for Zn-air batteries (ZAB), and FeCoNC@-850-5 had higher open-circuit voltage (OCV), power density, and specific capacity. These findings demonstrate that the catalyst possesses excellent catalytic activity and promising application prospects, providing a new perspective for the design of efficient oxygen reduction catalysts based on the coupling of bimetallic alloys and N-doped carbon materials.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 21
·7778-7786
·
IF 6.482
Wei Wei,Yongya Zhang,Lei Liang,Kefeng Wang,Qingfeng Zhou,Yanli Zhou,Hua Wang
Metal germanium (Ge) with a high theoretical capacity of 590 mA h g−1 is regarded as a promising anode material for sodium ion batteries, but it suffers from a fast capacity decay problem due to the serious agglomeration of Ge particles caused by the drastic volume change during the sodiation/desodiation process. Constructing highly dispersed ultrafine Ge nanoparticles is a possible way to address this problem. However, reported methods to obtain highly dispersed metal nanoparticles encountered problems of poor electrochemical activity or non-uniform particle size. In this work, we proposed a new in situ confined polymerization method for preparing highly dispersed Ge quantum dots (QDs). Due to the high dispersion of Ge QDs in carbon frameworks derived from poly(ionic liquid) networks, the obtained Ge@C nanocomposite could effectively avoid the agglomeration of Ge particles. When applied as the anode material for sodium ion batteries, the Ge@C nanocomposite shows ultra-long cycle life and high rate capability. At a current density of 1500 mA g−1, the Ge@C electrode could display a high capacity of 201 mA h g−1 after 5000 cycles. This method could be extended to prepare other highly dispersed metal nanoparticles and achieve fairly efficient electrode materials for new-type secondary batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Mingxia Song,Bofeng Zhang,Ziwei Zhai,Sibao Liu,Li Wang,Guozhu Liu
Atomically dispersed metal catalysts can maximize the utilization of metals and provide unique chemical properties for catalytic reactions. However, the stabilities of high-loading metal clusters on solid supports are still under dispute, because small clusters are prone to agglomerate into larger particles at high temperature. Here, we prepared thermally stable highly dispersed Pt species immobilized by bridging Zn2+ sites and silanol groups (Si-OH) on self-pillared silicalite-1 zeolite nanosheets (SP-S-1). The rotationally overgrown zeolite sheet-like structure provided a high specific surface area and abundant Si-OH, which favored atomically dispersed active sites with ZnOx-Si nanoclusters. The as-prepared PtZn/SP-S-1 exhibited a high specific activity of 1.23 molC3H6·gcatal–1·h–1 at 580 °C with propylene selectivity up to 99%. Moreover, no obvious deactivation was observed after 90 h on stream under a weight hourly space velocity of 15 h–1. The self-pillared nanosheet-supported metal catalysts provide prospective guidance for high-temperature catalysis.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2017
·
IF 3.33
Yingji Song,Shaodan Xu,Fei Ling,Panpan Tian,Tao Ye,Deqing Yu,Xuefeng Chu,Yingzi Lin,Xiaotian Yang,Junhong Tang
Here we reported the synthesis of Al sites with ultra-high dispersion on anatase by an atomic layer deposition (ALD) method (ALD-Al/TiO 2 ), which exhibits Brønsted acidity and satisfactory activity in the dehydration of alcohols, a key step in the deoxygenation of biomass. More importantly, the ALD-Al/TiO 2 catalyst has good stability, which is sintering-resistant and gives constant catalytic performances after treatments at high temperature.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Jun Li,Peng Ye,Jia Fang,Manye Wang,Deming Wu,Aihua Xu,Xiaoxia Li
Manganese oxide octahedral molecular sieves (OMS-2) supported CuO catalysts were synthesized, characterized and used in the removal of Acid Orange 7 (AO7) in aqueous solution by an oxidation process involving peroxymonosulfate (PMS). It was found that the CuO species were highly dispersed in OMS-2 with a high ratio of easily reduced surface oxygen species. The synergetic effect between CuO and OMS-2 significantly improved the dye degradation rate and catalytic stability, compared with CuO, OMS-2 and supported CuO on other materials. About 97% of the dye was removed within 15 min at neutral solution pH by using 0.2 g/L of CuO/OMS-2 and PMS. The effect of initial solution pH, PMS concentration, reaction temperature and CuO content in the composites on AO7 degradation was also investigated. Mechanism study indicated that SO 4 − radicals generated from the interaction between PMS and Mn and Cu species with different oxidation states, mainly accounted for the degradation.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Junpeng He,Ruiqing Zhang,Xi Chen,Bofeng Zhang,Guozhu Liu
Active fuel cooling is an effective way to overcome the thermal barrier for hypersonic flight. Pt-based nanofluid catalysts are effective in enhancing the chemical heat sink of endothermic hydrocarbon fuels (EHFs) by facilitating a catalytic dehydrogenation-cracking reaction. However, highly-dispersed Pt nanoparticles often face the problem of poor thermal stability in nanofluids. In this work, a NaH-assisted deprotonation method was applied to synthesize N-heterocyclic carbene (NHC)-capped highly-dispersed Pt nanoparticles (Pt@NHC14). The average size of the Pt nanoparticles in optimized Pt@NHC14 was 2.4 nm. Pt@NHC14 exhibited a high heat sink of 3.80 MJ/kg at 725 °C in the quasi-homogeneous conversion of decalin, which was 10% higher than Pt@ILs14 without a deprotonation strategy. This could be ascribed to the dehydrogenation process being promoted, which was verified by a hydrogen yield of 9.5% on highly dispersed Pt of Pt@NHC14, and that is 46% higher than that of Pt@ILs14. This research synthesizes N-heterocyclic carbene-capped highly-dispersed Pt nanoparticles and provides valuable insights into the strong endothermic technology.
研究领域:
材料科学
·
化学工程
·
航空航天工程
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2016
·Vol. 6
·期 9
·134
·
IF 2.964
Songbai Qiu,Ying Xu,Yujing Weng,Longlong Ma,Tiejun Wang
A series of MCM-41 supported Ni catalysts with high metal dispersion was successfully synthesized by simple co-impregnation using proper ethylene glycol (EG). The acquired Ni-based catalysts performed the outstanding hydrogenolysis activity of guaiacol. The effects of the synthesis parameters including drying temperature, calcination temperature, and metal loading on the physical properties of NiO nanoparticles were investigated through the use of X-ray diffraction (XRD). The drying temperature was found to significantly influence the particle sizes of NiO supported on MCM-41, but the calcination temperature and metal loading had less influence. Interestingly, the small particle size (≤3.3 nm) and the high dispersion of NiO particles were also obtained for co-impregnation on the mixed support (MCM-41:HZSM-5 = 1:1), similar to that on the single MCM-41 support, leading to excellent hydrogenation activity at low temperature. The guaiacol conversion could reach 97.9% at 150 °C, and the catalytic activity was comparative with that of noble metal catalysts. The hydrodeoxygenation (HDO) performance was also promoted by the introduction of acidic HZSM-5 zeolite and an 84.1% yield of cyclohexane at 240 °C was achieved. These findings demonstrate potential applications for the future in promoting and improving industrial catalyst performance.
研究领域:
催化化学
·
能源化学
·
材料化学
·
工业催化
·
生物质转化
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2017
·
IF 0
Yirui Shen,Pingping Jiang,Jian Zhang,Gang Bian,Pingbo Zhang,Yuming Dong,Weijie Zhang
Highly dispersed Molybdenum (VI) incorporated hollow mesoporous silica catalyst was facilely synthesized with a selective etching strategy and then followed with a modified immersion method. Firstly, hollow mesoporous silica spheres were obtained from solid silica spheres with the interaction of cetyltrimethyl ammonium bromide (CTAB) and Na 2 CO 3 . Then the catalytic sites were loaded by modified and direct immersion methods as comparison. The catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N 2 adsorption/desorption and X-ray photoelectron spectra (XPS). The reactivity of the catalysts was also detected under the same condition in olefin epoxidation. Compared with these two immersion methods, modified method exhibited the best turnover number of 3873 at 6 h with a better reactivity and textural properties than direct one. Highly dispersed molybdenum indeed brought excellent activity and high stability. The conversion could reach 100% with a selectivity above 99% after 12 h. And the catalyst still had a conversion above 86% and a selectivity above 93% after five runs. More importantly, this modified immersion method could also be widely used in the preparation of catalysts as a simple but efficient way.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
Applied Sciences-Basel
·
2019
·Vol. 9
·期 13
·2619
·
IF 2.217
Tao Li,Shaopeng Zeng,Yaxiong Ji,Boxu Shen,Zhuangmiao Wang,Hong Zhong,Shifeng Wang
To eliminate the negative impacts of waste stone powder that arises from stone processing, the waste was recycled into aerated bricks with a porous structure that exhibited exceptional properties when applied in buildings. However, the pores easily absorb rainwater and dust, causing performance degradation and mold growth inside. In this paper, we have developed through hydrothermal reactions an environmentally friendly aqueous suspension, containing homemade highly dispersive TiO2nanoparticles modified with super-hydrophobic groups on the surface. The suspension was coated onto the aerated bricks, creating a super-hydrophobic surface with a highly textured hierarchical structure. A large contact angle of 146° tested on the surface and negligible water absorption for 24 h immersion demonstrate the excellent water proofing performance, holding a great promise for large scale applications in construction and buildings.Keywords:aerated brick;waste recycling;hydrophobic;surface modification;TiO2nanoparticle;highly dispersive
研究领域:
建筑材料科学
·
环境科学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Gui-lin Zhuang,Yi-fen Gao,Xiang Zhou,Xin-yong Tao,Jian-min Luo,Yi-jing Gao,Yi-long Yan,Pei-yuan Gao,Xing Zhong,Jian-guo Wang
Herein we report a facile bottom-up strategy to prepare highly dispersed supported Co 3 O 4 on N-doped Porous Carbon (NPC). Specifically, ZIF-67 (ZIF = Zeolitic Imidazolate Frameworks) microcrystals firstly grow on benzoic acid modified covalent organic framework (BFC), resulting in ZIF-67/COF composite. Subsequently, highly dispersed Co 3 O 4 /NPC was obtained via the calcination of ZIF-67/COF. Interestingly, high dispersion of supported Co 3 O 4 is dominated by homogeneous distribution of benzoic acid auchoring on nanoporous COF . More notably, largely triggered by the porosity and confining effect of COF , the resultant Co 3 O 4 /NPC features highly active crystal plane and a large specific surface area of 228.0 m 2 /g. Furthermore, the oxygen evolution reaction (OER) measurement results demonstrated that highly dispersed Co 3 O 4 /NPC features good catalytic activity (330 mV overpotential at 10 mA.cm −2 , 79 mV.dec −1 Tafel slope and mass activity of 130 A.g −1 at overpotential of 400 mV) and durable stability, superior to currently available counterparts. Moreover, Li-ion battery (LIB) tests also showed high reversible capacity (785 mA.h.g −1 at 500 mA.g −1 ) as well as excellent cycling stability and rate performance. Furthermore, Density functional theory (DFT) calculation results demonstrated that these superior OER properties can be attributed to the geometrical and electronic effects of Co 3 O 4 /NPC on activation and adsorption/desorption of reaction species.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源存储
·
功能材料
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhixiu Yang,Xiu Wen,Xiaoxuan Guo,Yong Chen,Ruiping Wei,Lijing Gao,Xiaomei Pan,Jin Zhang,Guomin Xiao
The electrochemical CO 2 reduction to specific multi-carbon product on copper-based catalysts is subjected to low activity and poor selectivity . Herein, catalyst structure, morphology, and chemical component are systematically studied for bolstering the activity and selectivity of as-prepared catalyzers in this study. Dendritic fibrous nano-silica spheres favor the loading of active species and the transport of reactant from the central radial channel. Cu/DFNS with high dispersion active sites are fabricated through urea-assisted precipitation way. The coexistence of Cu(I)/Cu(II) induces a close combination of Cu active sites and CO 2 on the Cu/DFNS interface, promoting the CO 2 activation and C C coupling. The Cu–O–Si interface (Cu phyllosilicate) can improve CO 2 and CO attachment. Cu/DFNS show the utmost Faradaic efficiency of C 2 H 4 with a value of 53.04% at −1.2 V vs. RHE. And more importantly, in-situ ATR-SEIRAS reveals that the C C coupling is boosted for effectively producing C 2 H 4 as a consequence of the existence of *CO L , *COOH, and *COH intermediates. The mechanism reaction path of Cu/DFNS is inferred to be *CO 2 → *COOH → *CO → *CO*COH → C 2 H 4 . Our findings will be helpful to gain insight into the links between morphology, texture, chemical component of catalyzers, and electrochemical reduction of CO 2 , providing valuable guidance in the design of more efficient catalysts.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）