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Desalination and Water Treatment · 2024 · IF 1

Enhanced anti-fouling property of poly(vinyl chloride) membrane by blending poly(N-acryloylmorpholine)-grafted ZrO2 nanoparticle

Xiang Shen,Tiande Xie,Jiangang Wang,Fan Wang

In this work, poly(N-acryloylmorpholine)-grafted ZrO 2 nanoparticles (ZrO 2 -g-PACMO) were directly blended with poly(vinyl chloride) (PVC) to prepare a hybrid membrane via the phase inversion method. In addition, the effects of ZrO 2 -g-PACMO and ZrO 2 nanoparticles on the structure and performance of resultant PVC membranes were comparatively investigated. The results indicated that the PVC/ZrO 2 -g-PACMO membrane exhibited a large macroviod of cross-section and a rough membrane surface. During membrane formation, the hydrophilic PACMO chains were preferably enriched onto the membrane surface, leading to the enhancement of surface hydrophilicity and the reduction of adhesion force between protein and membrane surface. The amount of adsorbed bovine serum albumin (BSA) on the poly(vinylidene fluoride)/ZrO 2 -g-PACMO decreases about 73% and 48% respectively, compared with original PVC and PVC/ZrO 2 membranes. Cycle filtration of pure water and BSA solution (0.5 g/L) confirmed that the total and irreversible membrane fouling were remarkably suppressed after incorporating ZrO 2 -g-PACMO into PVC membrane. Although the original ZrO 2 nanoparticle was also found to improve the protein fouling resistance of PVC membrane, there was a fatal limitation that the original ZrO 2 exhibited an agglomeration tendency during the membrane formation. The outcomes of the present work demonstrate that the synthesized ZrO 2 -g-PACMO nanoparticles have the potential for the design and preparation of anti-fouling PVC membrane.

研究领域: 材料科学 · 膜技术 · 化学工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2020 ·Vol. 138 ·期 11 ·49992 · IF 2.52

Sulfonated polystyrene brushes grafted onto magnetic nanoparticles as recoverable catalysts for efficient synthesis of ethyl N-phenylformimidate

Xiaoying Wang,Lili Wang,Bingyan Sun,Xiaomeng Chu,Xuteng Xing,Shaojie Liu,Erjun Tang

In this work, the sulfonated polystyrene brushes were grafted onto magnetic nanoparticles to obtain recoverable catalysts for efficient synthesis of ethyl N-phenylformimidate. First, the surface modification of Fe 3 O 4 with a particle size of about 10 nm was performed with the silane coupling agent of vinyl triethoxysilane (SG-151) to obtain Fe 3 O 4 with carbon–carbon double bonds on the surface (SG-Fe 3 O 4 ). Subsequently, SG-Fe 3 O 4 , styrene (St) and chloromethyl styrene (CMSt) were polymerized to obtain the magnetic chloromethylated polystyrene sphere (SG-Fe 3 O 4 @PS-Cl) with core-shell structure by solution copolymerization. Using St as monomer and SG-Fe 3 O 4 @PS-Cl as macromolecular initiator, the magnetic polystyrene brush of SG-Fe 3 O 4 @PS-PSt was obtained by activated regenerated electron transfer catalyst atom transfer radical polymerization. Finally, SG-Fe 3 O 4 @PS-PSt was sulfonated with sulfuric acid to form a magnetic sulfonated polystyrene brush of SG-Fe 3 O 4 @PS-PSH. SG-Fe 3 O 4 @PS-PSH was used as a recoverable acid catalyst to synthesize ethyl N-phenylformimidate. Due to the high loading of the sulfonic acid group of this catalyst, its added amount was lower than other solid acids such as p-toluenesulfonic acid. The results showed that the catalytic performance of SG-Fe 3 O 4 @PS-PSH was better than p-toluenesulfonic acid and commercial macroporous sulfonic acid resin. The external magnetic field can directly recover SG-Fe 3 O 4 @PS-PSH, simplifying the recovery of catalyst and reducing the catalyst loss. After recycling, the yield of ethyl N-phenylformimidate was not significantly decreased.

研究领域: 材料科学 · 催化化学
✓ 已验证 DOI 高影响因子
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MICROPOROUS AND MESOPOROUS MATERIALS · 2019 · IF 4.182

Designing ordered composites with confined Co–N/C layers for efficient pollutant degradation: Structure-dependent performance and PMS activation mechanism

Junmei Luo,Shufeng Bo,Qingda An,Zuoyi Xiao,Haisong Wang,Weijie Cai,Shangru Zhai,Zhongcheng Li

Rational design of ordered catalytic composites with high performance and facile preparation method for environmental remediation still remains a tremendous challenge. For this vision, ordered composites with confined cobalt intercalated N/C layers (Co–N/C) were successfully prepared via carbonizing a mixture of cobalt species, histidine (His) and zirconium-containing SBA-15 (ZS) utilizing a simple non-solvent method. Taking the confinement effect and inherent hydrophilic groups (Si–OH) of mesoporous silica as the foothold, the strong Co 2+ /N or Co 2+ /O coordination (Co 2+ (–COO - or –NH 2 ) 2 and Co 2+ (–O - ) 2 ) and silica/His or His/His adhesive/cohesive interactions endowed the Co-based catalyst with optimal interfacial properties , cycling stability and magnetic separability for degradation of several pollutants (phenol, antibiotics and dyes). The degradation efficiency of Co@NC-ZS-700 for bisphenol A was superior to Co-ZS-700, NC-ZS-700 and Co@NC-SBA-700 due to the flaky structure with confined Co–N/C layers, which could achieve 95.0% within 20 min. In addition, the catalyst could still degrade more than 84.4% bisphenol A after five consecutive reactions. Based on the characterization analysis, tested active species (SO 4 •– , • OH and 1 O 2 ) and degradation products, double-process activation mechanism and degradation pathways were plausibly proposed (radical and non-radical processes). Additionally, various influencing factors, including carbonization temperature, amount of cobalt species, peroxymonosulfate (PMS)/catalyst dosage, pH value, coexisting ions and real water environment, were also systematically studied. This work might pave a feasible way for contaminant treatment utilizing ordered mesoporous silica composites with diffusion promoted channels involved under aqueous systems.

研究领域: 环境科学 · 催化化学
✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF CATALYSIS · 2022 · IF 12.92

Unveiling the highly disordered NbO6 units as electron-transfer sites in Nb2O5 photocatalysis with N-hydroxyphthalimide under visible light irradiation

Kaiyi Su,Chaofeng Zhang,Yehong Wang,Jian Zhang,Qiang Guo,Zhuyan Gao,Feng Wang

ABSTRACT Although different NbO x units are present in Nb 2 O 5 -based catalysts, the correlations between these structures and activity remain unclear, which considerably hinders the further development of Nb 2 O 5 photocatalysis . Herein, we utilized N- hydroxyphthalimide (NHPI) as the probe molecule to distinguish the role of different NbO x units in the activation of C–H bond under visible light irradiation. With the addition of NHPI, Nb 2 O 5 catalysts with highly disordered NbO 6 units exhibited higher activities than that with slightly disordered NbO 6 units (419–495 vs . 82 μmol·g −1 ·h −1 ) in photocatalytic selective oxidation of ethylbenzene . Revealed by Raman spectra, electron paramagnetic resonance spectra, and transmission-electron-microscopy images, highly disordered NbO 6 units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI, promoting the generation of phthalimide- N -oxyl (PINO) radicals for the enhanced conversion of ethylbenzene under visible light irradiation. This study provides guidance on the role of local NbO x units in Nb 2 O 5 photocatalysis.

研究领域: 材料科学 · 催化化学
✓ 已验证 DOI 高影响因子
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RSC Advances · 2016 ·Vol. 6 ·期 10 ·7902-7907 · IF 3.289

Strong base pre-treatment for colorimetric sensor array detection and identification of N-methyl carbamate pesticides

Sihua Qian,Yumin Leng,Hengwei Lin

Colorimetric sensor arrays demonstrate numerous superior features in chemo- and bio-sensing, but they are generally not applicable to less-reactive analytes. Based on the findings that N-methyl carbamate pesticides could be decomposed into reactive phenols in basic media, herein, a novel strategy of strong base pre-treatment was developed and employed for the colorimetric sensor array detection and differentiation of the N-methyl carbamate pesticides in an indirect manner. With the use of five inexpensive and commercially available phenol responsive indicators, such a colorimetric sensor array can be facilely fabricated. Classification analysis (e.g. hierarchical clustering analysis (HCA) and principal component analysis (PCA)) reveals that the as-fabricated sensor array has an extremely high dimensionality and, consequently, exhibits excellence in discriminating a variety of N-methyl carbamates from other types of pesticides and potential interferants, and further identifying them exactly from each other. Moreover, semi-quantitative detection could also be achieved through combining HCA/PCA, recognition patterns, and corresponding fitting curves. Overall, the as-developed method exhibits high selectivity and sensitivity, good anti-interference, simultaneous detection and identification capability for each of the N-methyl carbamate pesticides, and potential applicability in real samples. Most importantly, this study demonstrates that pre-treatment strategies are very effective in expanding the range of applications of colorimetric sensor array methodology to less-reactive analytes.

研究领域: 分析化学 · 环境科学 · 农业科学
✓ 已验证 DOI 高影响因子
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ACS Omega · 2019 · IF 2.584

Effect of Metal Precursors on the Performance of Pt/SAPO-11 Catalysts for n-Dodecane Hydroisomerization

Lili Geng,Jianjun Gong,Guilong Qiao,Songshou Ye,Jinbao Zheng,Nuowei Zhang,Binghui Chen

Pt(NH3)4(NO3)2, Pt(NH3)4(Ac)2, (NH4)2PtCl4, and H2PtCl6 were used to prepare Pt/SAPO-11 catalysts to investigate the effect of Pt precursors on the hydroisomerization of n-dodecane. The catalyst derived from Pt(NH3)4(NO3)2 displays the best hydroisomerization activity and selectivity among these precursors. The hydroisomerization conversion of n-dodecane is affected by the platinum particle size, platinum dispersion, the location of platinum, and the valence state of platinum. The selectivity of n-dodecane is determined by the number of Brønsted acid sites and Pt crystal planes. These conclusions are verified by combining transmission electron microscopy, high-resolution transmission electron microscopy, hydrogen temperature programmed reduction, NH3-temperature programmed desorption, and Py-IR studies. The catalyst prepared with Pt(NH3)4(NO3)2 as the precursor exhibits the smallest platinum particle size and the highest platinum dispersion. Most of the platinum particles are supported on the external surface of SAPO-11 with the Pt(111) crystal face. Such a catalyst also possesses a suitable number of Brønsted acid sites and then displays the best catalytic performance. Obviously, the use of various precursors for the Pt-based catalyst can significantly affect the performance of Pt/SAPO-11 for the hydroisomerization of n-dodecane.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF CATALYSIS · 2021 · IF 8.271

Geometric and electronic effects on the performance of a bifunctional Ru2P catalyst in the hydrogenation and acceptorless dehydrogenation of N-heteroarenes

Fangjun Shao,Zihao Yao,Yijing Gao,Qiang Zhou,Zhikang Bao,Guilin Zhuang,Xing Zhong,Chuan Wu,Zhongzhe Wei,Jianguo Wang

The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N -heterocycles is a challenge. In this study, Ru 2 P/AC effectively promoted reversible transformations between unsaturated and saturated N -heterocycles affording yields of 98% and 99%, respectively. Moreover, a remarkable enhancement in the reusability of Ru 2 P/AC was observed compared with other Ru-based catalysts. According to density functional theory calculations, the superior performance of Ru 2 P/AC was ascribed to specific synergistic factors, namely geometric and electronic effects induced by P. P greatly reduced the large Ru-Ru ensembles and finely modified the electronic structures, leading to a low reaction barrier and high desorption ability of the catalyst, further boosting the hydrogenation and acceptorless dehydrogenation processes.

研究领域: 催化化学 · 材料科学 · 理论化学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Preparation of a novel silica-based N-donor ligand functional adsorbent for efficient separation of palladium from high level liquid waste

Hefang Liu,Shunyan Ning,Zengyuan Li,Shichang Zhang,Lifeng Chen,Xiangbiao Yin,Toyohisa Fujita,Yuezhou Wei

In this work, a novel silica-based N-donor ligand functional adsorbent (SiVpC) is prepared by in situ polymerization for the efficient separation of palladium from high level liquid waste (HLLW). The as-prepared SiVpC adsorbent is characterized by SEM-EDS, TGA, and BET. The effects of nitric acidity, SiVpC adsorbent dosage, time, temperature, and palladium ion concentration on the adsorption are investigated. Among the 12 typical fission product metal ions (Ru, Rh, La, Y, Pr, Ce, Sm, Nd, Gd, Eu, Zr, Mo) existing in HLLW, SiVpC adsorbent can selectively adsorb palladium ( SF Pd/other metals  = 137.6) in 0.5 M HNO 3 solution. The adsorptio kinetics of Pd(II) are consistent with the pseudo-second-order model, reaching equilibrium within 120 min. The maximum adsorption capacity is 38.4 mg/g in 0.5 M HNO 3 , and the adsorption process is consistent with the Langmuir model. The adsorbed palladium can be completely desorbed with 0.5 M HNO 3 -0.5 M Thiourea. Furthermore, SiVpC adsorbent remains good performance after five adsorption–desorption cycles, which indicates good reusability. The adsorption mechanism of SiVpC adsorbent on palladium is analyzed by FT-IR and XPS that N-containing functional groups on the ligand are coordinated with palladium, which is also further verified by DFT calculations. In addition, through the column chromatography separation system, SiVpC adsorbent can efficiently adsorb palladium from HLLW and the adsorbed palladium can be desorbed with 0.5 M HNO 3 -0.5 M thiourea solution, which has great application potential.

研究领域: 化学工程 · 环境科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Self-supported bifunctional electrocatalysts with Ni nanoparticles encapsulated in vertical N-doped carbon nanotube for efficient overall water splitting

Yu Cheng,Haoran Guo,Pengfei Yuan,Xinpan Li,Lirong Zheng,Rui Song

To satisfy the practical requirements of electrochemical water splitting, developing a flexible, effective and sustainable approach for scalable production of bifunctional electrocatalyst for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is a tremendous issue to be rationally addressed. Herein, a solid-state diffusion strategy with Ni foam and N-doped carbon layers is applied to prepare multi-interfacial, self-supported and N-doped carbon nanotube (NCNT) encapsulated Ni nanoparticles (NPs) array bifunctional electrocatalyst (NCNT-NP@NF). Prominently, this NCNT-NP@NF is scalable to meet the application requirements and can be used as a binder-free electrode for direct the water splitting. The optimal sample demonstrate outstanding HER/OER performance in 1.0 M KOH, with low overpotential ( η 10 ) at 10 mA cm −2 during HER (96.1 mV) and OER (240 mV) process, which is extremely superior to the most reported metal-based electrocatalysts and even better than commercial IrO 2 (400 mV at 10 mA cm −2 for OER). Strikingly, when these bifunctional electrocatalysts are employed in a dual-electrode electrolyzer for water splitting, the NCNT-NP@NF only needs cell voltage of 1.54 V to drive overall water splitting in 1.0 M KOH, and displays excellent long-term stability (150 h for water splitting). Moreover, experiments combined with density functional theory (DFT) calculations clarify that the remarkable electrochemical activity and stability are mainly attribute to the synergistic effect of the uniform distribution of Ni NPs, heteroatomic doping, as well as district confinement effect of NCNT leading to enhanced electronic multi-interfacial transmission, all these factors co-accelerate electrocatalytic kinetics. Accordingly, this solid-state diffusion method possesses a favorable potential to construct a multi-interfacial and self-supported electrocatalysts in the fields of sustainable supply of clean energies.

研究领域: 电化学 · 材料科学 · 催化 · 能源材料 · 可持续能源
✓ 已验证 DOI 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2024 · IF 3.3

Minisci-Type Dehydrogenative Coupling of N-Heteroaromatic Rings with Inert C(sp3)–H Enabled by a Visible-Light-Catalyzed Intermolecular Hydrogen Atom Transfer Process

Jun-Feng Yang,Yun-Fei Liu,Lin-Lin Wei,Kai-Kai Qiao,Yan-Qiu Zhao,Lei Shi

The Minisci-type dehydrogenative coupling of N-heteroaromatic rings with inert C–H or Si–H partners via visible-light-catalyzed hydrogen atom transfer has been reported. This methodology allows the coupling reactions to be carried out in water as a solvent under air atmospheric conditions with visible-light illumination. A wide range of inert C–H and Si–H partners could be directly coupled with various N-aromatic heterocycles to deliver products in good to excellent yields.

研究领域: 有机化学 · 光化学
✓ 已验证 DOI PubMed 高影响因子
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ChemCatChem · 2017 ·Vol. 10 ·期 4 ·796-803 · IF 4.803

Controllable Synthesis of CoS2@N/S-Codoped Porous Carbon Derived from ZIF-67 for as a Highly Efficient Catalyst for the Hydrogen Evolution Reaction

Shi Feng,Xingyue Li,Jia Huo,Qiling Li,Chao Xie,Tingting Liu,Zhigang Liu,Zhenjun Wu,Shuangyin Wang

Graphical Porous carbon electrode : CoS 2 @N/S-codoped porous carbon is prepared through an electrodeposition–ZIF conversion–sulfuration strategy. The loading of active sites can be controlled easily by varying the electrodeposition time. The resulting material can be employed directly as a working electrode for the hydrogen evolution reaction and shows an excellent catalytic activity and stability. A convenient, controllable method to fabricate an electrode is necessary to achieve the practical application of a hydrogen evolution reaction (HER) catalyst. In this work, an electrodeposition–ZIF conversion–sulfuration strategy is developed to produce a CoS 2 @N/S-codoped porous carbon (CoS 2 @NSC/CFP) to drive the HER efficiently. CoS 2 @NSC/CFP was prepared by the electrodeposition of Co(OH) 2 on a carbon fiber paper followed by conversion into ZIF-67 and subsequent sulfuration with sulfur. The loading of electroactive components can be controlled easily in the range of 0.7–10.0 mg cm −2 by varying electrodeposition time from 5 min to 2 h. The resulting material can be employed directly as a working electrode for the HER and it shows an excellent catalytic activity and stability with an overpotential of 95 mV at 10 mA cm −2 and 158 mV to reach 100 mA cm −2 in an acidic medium. The high efficiency is related intimately to the high dispersion of ultra-small CoS 2 nanoparticles, heteroatom-codoping, and the 3 D porous network configuration of the carbon fiber paper.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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Industrial Chemistry & Materials · 2024 · IF 0

Elongated Fe–N–C containing trace atomic Co dopants for high power density PEMFCs

Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu

Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.

研究领域: 电化学 · 催化 · 能源材料 · 燃料电池 · 纳米技术
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