DALTON TRANSACTIONS
·
2025
·
IF 3.3
An-Ran Xue,Yang Hao,Cun-Wei Kang,Qing Cai,Jia-Shen Li,Kun Dong,Songdong Ding,Yuan-Ru Guo,Qing-Jiang Pan
A synthetic strategy was developed to fabricate large surface-area, hierarchical structured and anti-photocorrosion CdS composite starting from CdCO3 with the assistance of nitrogen-doped carbon dots (NCDs). Initially, NCDs were coated over the CdCO3 surface. Once triggering the reaction, NCDs electrostatically enriched S2– ions and meticulously regulated the interface of the newly-formed CdS with CdCO3 to facilitate mass transfer. This led to entire conversion to the composite NCDs/CdS, where CdS exhibited a hierarchical nanoflake-layer-particle architecture. Various characterizations indicate that NCDs loaded on CdCO3 dynamically promoted the formation of cubic-phase CdS. The unique morphology enlarged the specific surface area to 62.1 m2 g–1. Of the synthesized samples, NCDs/CdS-60 achieved a hydrogen production rate as large as 2.27 mmol g–1 h–1, which is almost 11-fold higher than CdS prepared without adding NCDs. Notably, the component of NCDs suppressed the hole-induced photocorrosion of CdS during the photocatalytic reaction and extended the catalyst’s service life.
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MOLECULES
·
2023
·Vol. 28
·期 8
·3542
·
IF 4.6
Qing Liu,Chao Yan,Yan Wang
Applications of submicron-scale particles are of rising interest in separation science due to their favorable surface-to-volume ratio and their fabrication of highly ordered structures. The uniformly dense packing beds in columns assembled from nanoparticles combined with an electroosmotic flow-driven system has great potential in a highly efficient separation system. Here, we packed capillary columns using a gravity method with synthesized nanoscale C18-SiO2particles having diameters of 300–900 nm. The separation of small molecules and proteins was evaluated in the packed columns on a pressurized capillary electrochromatography platform. The run-to-run reproducibility regarding retention time and peak area for the PAHs using a column packed with 300 nm C18-SiO2particles were less than 1.61% and 3.17%, respectively. Our study exhibited a systematic separation analysis of small molecules and proteins based on the columns packed with submicron particles combined with the pressurized capillary electrochromatography (pCEC) platform. This study may provide a promising analytical approach with extraordinary column efficiency, resolution, and speed for the separation of complex samples.Keywords:submicron scale particles;pressurized capillary electrochromatography;separation
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Nano Research
·
2023
·Vol. 16
·期 5
·6568-6576
·
IF 9.9
Zhang Genrui,Li Xiaojing,Li Na,Wu Tingting,Wang Lei
Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites. Herein, 2D porous NiCo oxyphosphide (NiCoOP) was synthesized for the first time and coupled with graphitic carbon nitride (g-C 3 N 4 ) nanosheets to form 2D/2D heterojunctions via an in-situ phosphating method. The optimal 4 wt.% 2D/2D NiCoOP/g-C 3 N 4 (OPCN) photocatalyst achieves a hydrogen evolution rate of 1.4 mmol·h −1 ·g −1 , which is 33 times higher than that of pure g-C 3 N 4 . The greatly improved photocatalytic performance of the composite photocatalysts could be attributed to the formation of interfacial surface bonding states and sufficient charge transfer channels for accelerating carrier separation and transfer and the porous structure of NiCoOP nanosheets with abundant surface active sites for promoting surface reactions. Amazingly, the 2D/2D OPCN composite photocatalysts also exhibit superior stability during photocatalytic reactions. This study not only designs new noble-metal-free NiCoOP/g-C 3 N 4 composite photocatalysts but also provides a new sight in fabricating face-to-face 2D/2D heterojunctions for their application in energy conversion areas.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Hengye Li,Xingwei Han,Lin Zhang,Wenjie Yu,Wenwen Bie,Meijie Wei,Zhongxia Wang,Fenying Kong,Wei Wang
Herein, β-cyclodextrin-containing hybrid polymers (P1, P2 and P3) were prepared through crosslinking partially benzylated β-cyclodextrin (PBCD) by octavinylsilsesquioxane (OVS). P1 stood out in screening studies and the residual hydroxyl groups of PBCD was sulfonate-functionalized. The obtained P1-SO 3 Na showed greatly enhanced adsorption towards cationic MPs and maintained the excellent adsorption performance towards neutral MPs. The rate constants ( k 2 ) of cationic MPs upon P1-SO 3 Na were 9.8–34.8 times larger than those upon P1. The equilibrium uptakes of the neutral and cationic MPs upon P1-SO 3 Na were above 94.5 %. Meanwhile, P1-SO 3 Na demonstrated appreciable adsorption capacities, excellent selectivity, effective adsorption of mixed MPs at environmental levels and good reusability. These results confirmed the great potential of P1-SO 3 Na as effective adsorbent to remove MPs from water.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Rongqing Chen,Yunjia Liu,Jinlan Weng,Hua Huang,Xiaoying Gao,Zhipeng Wang,Jian Liu
The alteration of agricultural wastes into novel adsorbents can stimulate their scalability in realistic application, showing great economic and environmental advantages. Here, we proposed a strategy to engineer rice husk (RH) with microporous melamine-formaldehyde networks (MFNs) resins and the utilization for dynamic removal of organic micropollutants rapidly and efficiently. was pre-treated to acquire attractive surface and unique hierarchical porosity, endowing with surface functionalization and essential filtering properties. MFNs can be uniformly generated in-situ on the fully exposed cellulose backbones of the pre-treated RH. MFNs granules functionalized RH (RH@MFNs) exhibited high removal efficiencies over 90% within 30 min for the adsorption of hazardous organic compounds ( e.g., phenolic and antibiotic micropollutants) in static tests. Experiment results and density functional theory (DFT) simulation revealed that the synergy of hydrogen bonding, π-πinteraction, and micropore preservation dominates the adsorption. Further dynamic adsorption experiments showed that the removal efficiency and equilibrium removal capacity towards bisphenol A by RH@MFNs packed bed up-flow column were 2.6 and 67 times higher than that of raw RH, respectively. The column adsorption fits well with the Thomas model and bed depth service time (BDST) kinetic model. The inherent macropores inside RH and the roughness caused by the spiky structures and mesopores outside RH, as well as the accumulated MFNs granules, can lead to local turbulence of water flow around RH@MFNs, enabling fast and efficient adsorption. This sustainable and cost-effective preparation of RH-based adsorbents sheds light on the rational design of biomass waste adsorbents for realistic wastewater.
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JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 30
·期 1
·1-8
·
IF 3.061
Qu Shuzhang,Li Haokun,Song Jianhui,Wang Wei
A series of half-metallocenes of the type Cp’TiCl 2 (L) [Cp’ = Cp, L = naphthalen-1-yloxy ( 1a ), (2,4-dichloronaphthalen-1-yl)oxy ( 1b ), naphthalen-2-yloxy ( 1c ); Cp’ = C 5 Me 5 (Cp*), L = naphthalen-1-yloxy ( 2a )] are synthesized and well characterized. Using these complexes as catalysts for the polymerization of styrene in the presence of methylaluminoxane (MAO) cocatalyst, highly syndiotactic polystyrene can be obtained. The effects of anionic ligands, cyclopentadienyl, and polymerization conditions, such as Al/Ti molar ratio and polymerization temperature, on both the catalytic activity and the molecular weights of the resulted polymer are discussed. Higher polymerization temperature gives higher activity, but the obtained polymer has lower molecular weight. The higher Al/Ti ratio gives higher activity, while the molecular weight of the polymer increases with the increase of MAO amount in a certain range. This may indicate that the transfer to aluminum is not the main chain transfer mode of this polymerization. The activity of Cp* catalyst is higher than that of Cp catalyst, which indicates that the substituted methyls provides the stability of active center. Moreover, the molecular weight of the polymer obtained by the former is significantly higher than that of the latter, which indicates that the chain transfer reaction is inhibited by methyls on Cp ligand. Naphthyloxy ligands with different structures have no significant difference in polymerization activity and molecular weight of polymers.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 4.446
Songyan Qin,Xiaolong Liu,Wujuan Lv,Jie Hu,Xin Huang,Lixin Zhao
This study describes the degradation of α-naphthol by magnetic biogenic manganese oxides (M-BMnOx) prepared using Pseudomonas putida strain QSY-1 and magnetic nanoparticles (MNPs) added to the medium. The influence of various reaction parameters, such as pH, temperature, and initial α-naphthol concentration, was systematically investigated. Based on a complete process dynamics model and the initial kinetic analysis, the degradation rate of M-BMnOx was shown to be faster than that of biogenic manganese oxides (BMnOx). The α-naphthol removal rate during the recycling of M-BMnOx also reached 100 % within the fourth cycle. The reaction pathway of α-naphthol was determined. Analyses of the α-naphthol degradation solution showed that M-BMnOx have superior removal efficiency compared with that of BMnOx, which makes it a potentially reliable technique for degrading high concentrations of α-naphthol wastewater.
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CHEMPHYSCHEM
·
2022
·Vol. 24
·期 6
·e202200845
·
IF 3.52
Ting Wang,Haocheng He,Zihan Meng,Siran Li,Ming Xu,Xueting Liu,Yuan Zhang,Mei Liu,Ming Feng
Graphical A novel “mixed-valent cobalt modulation” strategy is presented to enhance the electrocatalytic oxygen evolution reaction (OER) performance of perovskite LaCoO 3 (LCO). An optimized catalyst with 1.98 % Co 2+ /Co 3+ exhibits a significant magnetic-field enhancement for the OER activity. Extensive efforts to enhance the oxygen evolution reaction (OER) catalytic performance of transition metal oxides mainly concentrate on the extrinsic morphology tailoring, lattice doping, and electrode interface optimizing. Nevertheless, little room is left for performance improvement using these methods and an obvious gap still exists compared to the precious metal catalysts. In this work, a novel “mixed-valent cobalt modulation” strategy is presented to enhance the electrocatalytic OER of perovskite LaCoO 3 (LCO) oxide. The valence transition of cobalt is realized by ethylenediamine post reduction procedure at room temperature, which further induces the variation of magnetic properties for LCO catalyst. The optimized LCO catalyst with Co 2+ /Co 3+ of 1.98 % exhibits the best OER activity, and the overpotential at 10 mA cm −2 current density is decreased by 170 mV compared pristine LCO. Impressively, the ferromagnetic LCO catalyst can perform magnetic OER enhancement. By application of an external magnetic field, the overpotential of LCO at 10 mA cm −2 can be further decreased by 20 mV compared to that of under zero magnetic field, which arises from the enhanced energy states of electrons and accelerated electron transfer process driven by magnetic field. Our findings may provide a promising strategy to break the bottleneck for further enhancement of OER performance.
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Materials Today Physics
·
2023
·
IF 11.5
Qi Xue,Zixin Ge,Zihan Yuan,Jiangtao Huang,Bin He,Yu Chen
The highly active, selective and stable anode electrocatalysts for the ethanol oxidation reaction (EOR) are extremely desirable for the application of direct ethanol fuel cells (DEFCs). Herein, one-dimensional Au core@AuPt 0·20 Rh 0.08 alloy shell nanowires (Au@AuPt 0·20 Rh 0.08 CS-NWs) with long aspect ratio and cross-linked network architecture are synthesized. For the EOR, Au@AuPt 0·20 Rh 0.08 CS-NWs display higher peak current density, better resistance to CO poisoning and more lasting stability compared with Au@AuPt 0.28 CS-NWs and commercial Pt black electrocatalyst, which can be attributed to the trimetallic synergistic effect between the Au, Pt and Rh atoms. Specifically, the Rh can promote the C–C bonds and adsorb OH ads while Au can change the electronic structure of Pt, endowing Pt with a high anti-poisoning ability to CO ads and promoting the complete oxidation of various C1 intermediate to CO 2 . This work provides an effective strategy for the rational construction of high-performance Pt-based EOR electrocatalysts by optimizing composition, morphology and architecture.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2023
·
IF 6
Yongdi He,Jinou Song,Jiuzhong Yang,Yuan Zhuang,Liang Qiu,Zhijun Li,Shubao Song,Jibiao Xie
An experimental study of 5% 1 -nitropropane (1-NP)-initiated cyclohexane pyrolysis was carried out in a flow reactor at 30 Torr (4.0 kPa) over a temperature range of 673–1273 K. The pyrolysis species were detected with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) technique. Pyrolysis species from m/z 15–106, including C 1 -C 8 hydrocarbons, CO, NO, NO 2 , CH 2 O, CH 3 OH and C 3 H 5 NO, were identified with near-threshold photoionization efficiency (PIE) spectra and quantified at different temperatures. The experimental results indicated that the addition of 1-NP obviously reduced the initial pyrolysis temperature of cyclohexane from 1048 to 1098–723 K, and caused the decreases of the initial formation temperatures for the species from cyclohexane pyrolysis. Almost all the high-temperature pyrolysis species in the mechanisms proposed in the literature were identified in the experiments. Based on the experimental results in this work and rate coefficients proposed in the literature, the primary pyrolysis mechanisms of cyclohexane in the presence of 1-NP were discussed. The 1-NP pyrolysis occurs at a lower temperature than the cyclohexane does, and produces HONO, NO 2 , C 3 H 7 , etc. It was demonstrated that cyclohexane was mainly consumed via the H-atom abstractions by H and OH attacks in this work and the cyclohexyl radical formed via H-atom abstractions mainly isomerized into 1-C 6 H 11 -6 radical, which further combines with H to form 1-C 6 H 12 .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2023
·
IF 2.2
Yuxin Sun,Ye Li,Jiajia He,Liuyun Chen,Hongbing Ji,Zuzeng Qin,Tongming Su
Ternary sulfide solid solutions have garnered great attention in photocatalytic water splitting due to their tunable electronic property, low cost, and sufficient light-absorption performance. Herein, a series of Mn x Cd 1 – x S samples with different Mn/Cd molar ratios were synthesized by solvothermal method and used for photocatalytic hydrogen production under visible light. The Mn 0.2 Cd 0.8 S and Mn 0.4 Cd 0.6 S are demonstrated to be the solid solutions, while Mn 0.6 Cd 0.4 S and Mn 0.8 Cd 0.2 S consist of Mn x Cd 1 – x S solid solution and MnS. In addition, the Mn 0.4 Cd 0.6 S exhibits the highest photocatalytic performance with the H 2 production rate of 185.95 μmol·h −1 , which is 4.7 times higher than that of CdS. Without cocatalyst, the quantum efficiency of Mn 0.4 Cd 0.6 S reaches 2.04% at 400 nm. In addition, the Mn 0.4 Cd 0.6 S solid solution also shows high stability during the photocatalytic H 2 production reaction. The effect of Mn/Cd molar ratio on the microstructure, band gap structure, and photocatalytic hydrogen production performance of Mn x Cd 1– x S was revealed systematically. The excellent photocatalytic H 2 production performance of Mn 0.4 Cd 0.6 S solid solution is mainly due to its enhanced reducing potential and high charge separation efficiency.
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