CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhefei Zhao,Xuyao Yao,Ruopeng Yu,Xingyu Luo,Minhao Chen,Xiangxiang Zhang,Yinghua Xu,Youqun Chu,Xinbiao Mao,Huajun Zheng
Electrocatalytic hydrodechlorination (EHDC) stands out as an economical and prospective technology for eliminating chlorinated organic pollutants. Single-atom catalyst engineering and metal-support interaction (MSI) offer the promising strategies for developing electrocatalysts with high atom utilization and reactivity. Herein, atomically dispersed palladium (Pd) anchored on the iron (Fe)-introduced nickel phosphide (NiFeP) support is reported. The prepared NiFeP-Pd electrode exhibits outstanding electrocatalytic activity in 4-CP removal efficiency (98.8 %) with an ultra-low dosage of Pd (0.0497 mg cm −2 ) and the highest reported MA value (446.01 min −1 g −1 ), surpassing Ni 2 P-Pd by 6.34 times. Experimental results combined with theoretical calculations suggest that the superior performance of NiFeP-Pd stems from the modulated support by Fe introduction, which not only enhances the generation of adsorbed atomic hydrogen species (H*), but also reduces the energy barrier of C-H formation on Pd sites by regulating the MSI. In addition, single-Pd-atom construction on NiFeP with good conductivity and large specific surface area makes the contributions as well.
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PROGRESS IN ORGANIC COATINGS
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2024
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IF 6.5
Beibei Chen,Wenquan Dong,Wenchao Shi,Xuanlin Li,Bi Yang,Yang Tong,Lin Zhang,Jianzhang Wang
Developing high-performance of organic solid lubricating coating is of great significance for extending the life of the moving systems/parts. Herein, the non-covalently modified h-BN nanosheets by graphene oxide (BNNSs/GO) were elaborately constructed to enhance the mechanical, friction and wear properties of epoxy nanocomposite coating. The microstructure feature and chemical composition of BNNSs/GO were determined by various spectroscopic techniques. The tribological performance of nanocomposite coatings were tested using ball-on-disc friction tester, and 440C stainless-steel ball with diameter of 8 mm was used as the counterface material. The GO nanosheets acted an active platform for BNNSs, which improved the dispersion of BNNSs and interface interaction with epoxy. The anchoring BNNSs could break the strong π-π, and van der Walls forces among GO nanosheets. The thickness of epoxy nanocomposite coatings was about 60 μm. And the epoxy-1.0 wt%BNNSs/GO demonstrated much higher hardness and elastic modulus than epoxy, increased by 112.62 % and 53.37 %, respectively. The coefficient of friction (COF) and wear rate of epoxy-1.0 wt%BNNSs/GO were the lowest, with a reduction of 89.7 % and 97.5 %, respectively. The synergistic lubricating mechanism of epoxy-BNNSs/GO coating was proposed, which could provide a new light on the design of high antifriction and wear resistance of organic nanocomposite coating.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2017
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IF 2.536
Huihui Li,Cailing Yang,Xinyue Zhu,Haixia Zhang
A simple ratiometric fluorescent sensor for fructose was presented. It consisted of 10-hydroxybenzo[ h ]quinoline (HBQ) which showed emission at 572 nm and 3-pyridylboronic acid (PDBA) whose complex with HBQ gave emission at 500 nm. The reaction of fructose with PDBA inhibited the complexation of HBQ with PDBA, resulting in the change of dual-emission intensity ratio. The sensor well quantified fructose in the range of 0.015–2.5 mM with detection limit of 0.005 mM. Besides, this sensor exhibited excellent selectivity and was successfully applied to fructose detection in food. This work provides a simple ratiometric sensing platform for sensitive and selective detection of fructose.
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CATALYSIS COMMUNICATIONS
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2024
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IF 3.4
Chenan Yang,Yi Liu,Ying Hu,Peng Wang,Yuling Yang,Shangxing Chen,Zongde Wang,Xiang Li
Catalytic valorization of biomass into high energy density fuels plays a vital role in order to achieve future carbon neutrality. Herein, a class of H-MZ-5 catalysts with different mesoporous pore structures and acid site properties were synthesized. Among them, HMZ-5 prepared with tetrapropylammonium bromide (TPABr) and hexadecyltrimethylammonium bromide (CTAB) as templating agents showed the most excellent catalytic activity and selectivity of α-pinene dimerization. Under optimal catalytic conditions, 100% α-pinene was converted with 89.6% selectivity to dimers. The efficient catalytic activity and affordability of the catalysts in this system make it promising for industrial applications.
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Catalysts
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2024
·Vol. 14
·期 4
·248
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IF 3.8
Xinyi Xing,Wanni Liu,Siquan Xu,Jianxiu Hao
H-Beta zeolite is a solid acid catalyst commonly utilized in the catalytic conversion of biomass resources. In this study, H-Beta zeolite was calcined at different temperatures (350, 550, 750, and 1000 °C) to explore the effects of high temperature-induced dealumination on its physicochemical properties and its catalytic ability to convert glucose into 5-hydroxymethylfurfural (HMF). It was shown that as the calcination temperature increased, the Si-O-Al bond of H-Beta zeolite was broken and its dealumination effect was enhanced. Dealumination led to the collapse of the framework of H-Beta zeolite and a reduction in the number of acid sites, which in turn reduced its catalytic performance and the efficiency of HMF formation from glucose. Furthermore, H-Beta zeolite exhibited an extraordinary catalytic ability for the production of HMF from carbohydrates. Using glucose and cellulose as substrates, superior HMF yields of 91% and 46%, respectively, were achieved under optimal reaction conditions. Further, calcination removes carbon deposits in the recovered H-Beta zeolite, but it affects the cycling stability of the catalyst. Meanwhile, the by-products formed during the synthesis of HMF from glucose catalyzed by H-Beta zeolite catalyst were also clearly detected.
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POLYMER
·
2024
·
IF 4.1
Zaoxia Wen,Liang Xu,Xingyu Liu,Linxuan Fang,Lianbin Wu
A novel method was developed for constructing cross-linked silsesquioxane, utilizing Q-type H-POSS as a precursor. The Piers-Rubinsztajn (P–R) like reaction of Q-type H-POSS was catalyzed by B(C 6 F 5 ) 3 , resulting in the production of a prepolymer containing partial Si–H. Upon heating at high temperature in air, the prepolymer transformed into an insoluble and infusible cross-linked polymer, named Cured poly(H-POSS). This polymer exhibited high thermostability, with a 5 % weight loss temperature ( T 5d ) of 709 °C and a residue of 92 % at 800 °C. Additionally, Cured poly(H-POSS) exhibited high transparency, with a transmittance of 90 % in the 400–800 nm wavelength range, and favorable dielectric properties, with a dielectric constant ( D k ) of 2.88 at 14 GHz.
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RARE METALS
·
2024
·
IF 9.6
Li Zhao-Yang,Zhao Wei-Jun,Sun Yu,Zhou Bing,Feng Yue-Zhan,Liu Chun-Tai
The pressing demand for ultrathin and flexible shields to counter electromagnetic interference (EMI) has sparked interest in Ti 3 C 2 T x MXene materials due to their exceptional electrical conductivity, tunable surface chemistry, and layered structure. However, pure Ti 3 C 2 T x MXene films often lack the mechanical properties required for practical engineering applications, and traditional reinforcement methods tend to reduce electrical conductivity. This work demonstrates an effective strategy to enhance the alignment and densely packed layered structure of Ti 3 C 2 T x MXene films by regulating the acidity and alkalinity of Ti 3 C 2 T x MXene aqueous solutions. This approach simultaneously improves mechanical strength and electromagnetic interference shielding effectiveness (EMI SE). Compared with original Ti 3 C 2 T x MXene films, MXene films modified with ammonia solution (NH 3 ·H 2 O) via OH − show a significant improvement in tensile strength (27.7 ± 1.9 MPa). Meanwhile, MXene films treated with hydrochloric acid (HCl) via H + reach an even higher tensile strength of 39 ± 1.5 MPa. Moreover, the EMI SE values of the treated MXene films increase significantly, each reaching 66.2 and 58.4 dB. The maximum improvements in EMI SE values for the acid- and alkali-treated samples are 17.9% and 4%, respectively. In conclusion, the simultaneous enhancement of mechanical strength and EMI shielding efficacy highlights the potential of acid- and alkali-treated Ti 3 C 2 T x MXene films for applications in ultrathin and flexible EMI shielding materials. Graphical abstract
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FUEL
·
2024
·
IF 6.7
Jun Zhang,Shuyue Liu,Shiyu Lu,Chunyuan Wang,Pingjuan Liang,Huan Yi,Mengjie Li,Laizheng Luo,Rong Wang,Guangming Jiang
Improving the utilization of hydrogen radicals (H*) is of great significance for effective Pd-mediated electrocatalytic hydrodechlorination (EHDC) in detoxifying chlorinated organic pollutants (COPs). However, the limited H* utilization by single Pd arises from its inadequate performance in adsorbing/activating COPs and inferior mass transfer of low-concentration COPs. In this study, an urchin-like yolk/shell TiO 2 spheres with mesoporous structure are developed for supporting Pd nanoparticles (Pd/U-TiO 2 ), which exhibits superior EHDC activity and selectivity for 2,4-DCP reduction. Notably, the prepared Pd/U-TiO 2 catalyst achieves a mass activity of 4.2 min −1 g Pd -1 and a specific activity of 1.94 min −1 mol Pd -1 when detoxifying 50 mg/L of 2,4-DCP at −0.85 V, surpassing the most reported catalysts. Furthermore, the Pd/U-TiO 2 catalyst consistently demonstrates higher H* utilization efficiency compared to single Pd, regardless of the 2,4-DCP concentration or reaction mode (batch or continuous-flow). This enhanced H* utilization efficiency is attributed to two key factors: the urchin-like and yolk/shell structure of U-TiO 2 enhances the mass diffusion of 2,4-DCP, and the strong interactions between Pd and U-TiO 2 generate electron-rich Pd species that enhance the adsorption and activation of COPs. Overall, this work highlights the synergistic effects of strong metal-support interactions and mass diffusion in enhancing atomic H* utilization. This study lays a significant experimental and theoretical foundation for designing efficient electrocatalysts for the detoxification of chlorinated organic pollutants and various other halogenated organic pollutants.
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JOURNAL OF PHYSICAL ORGANIC CHEMISTRY
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2012
·Vol. 26
·期 1
·23-29
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IF 1.963
Chang-Di Chen,Wen-Bing Sheng,Guo-Jun Shi,Can-Cheng Guo
The regioselective hydroxylation of the aromatic C–H bond on a series of naphthalenes with different β-substituent R (R = H, Me, Et, i -Pr, OMe, COOH, Br, etc.) was studied, and the substituent effect on the regioselectivity was investigated. The electron-donating substituent afforded the aromatic C–H bond hydroxylation at the 1α position with more than 80% selectivity, while the electron-withdrawing substituent afforded the aromatic C–H bond hydroxylation at the 4α position with more than 60% selectivity of β-substituted naphthalene hydroxylated with metachloroperbenzoic acid catalyzed by tetrakis(pentafluorophenyl)porphyrin manganese(III) chloride. The research showed that the steric and electronic effects of the substituent appeared to play a significant role in determining the regioselectivity, and the electronic effect was of more importance than the steric effect of the substituent in the current situation. The studies may provide additional proofs for the stepwise mechanism of the aromatic C–H bond hydroxylation through a cationic intermediate. Copyright © 2012 John Wiley & Sons, Ltd.
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MATERIALS RESEARCH BULLETIN
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2024
·
IF 5.3
Yu Chang,Jianan Zhang,Ivan S. Babichuk,Hailong Liu,Yijie Liu,Jian Yang
The release of ammonia (NH 3 ) in industry or daily life is harmful to human health. A gas sensor was developed using h -MoO 3 nanorods and graphene film to detect and eliminate this. The h -MoO 3 nanorods were first synthesized by chemical bath deposition using ammonium molybdate tetrahydrate (NH 4 ) 6 Mo 7 O 24 •4H 2 O and HNO 3 and then deposited on the graphene film transferred to SiO 2 /Si substrate by electrochemical bubbling method. Subsequently, gas-sensitive h -MoO 3 @Graphene composite films were prepared and analyzed using Raman, XRD, SEM, and UV–vis. The gas sensor's performance was evaluated to detect NH 3 at a room temperature concentration range of 1–60 ppm. Compared with graphene, the conductivity of the composite film with 10 mg/ml h -MoO 3 nanorods was increased by 40 % and the sensitivity increased by 10 times. The sensor h -MoO 3 @G-10 showed the best sensing performance to 1 ppm NH 3 . Sensor sensitivity, response and recovery time are 1.1 %, 46.8 s and 17.8 s.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Yu Gu,Zhiqiang Tao,Shujia Zhang,Xiaohui Wang,Hao Yan,Xinmei Liu,Lei Wang,Jun Xu,Hui Shi
Methane–propane coaromatization (MPCA) upgrades two abundant and inexpensive light alkanes into value-added aromatic products. While Ga-loaded MFI zeolites represent by far the most promising catalysts for MPCA reaction, they often contain a sizable portion of Ga species at the external surface of zeolites, which are remote from the Brønsted acid sites (BAS) within MFI pores and thus inefficient for MPCA. Here, we show that Ga can be introduced into MFI pores at fairly high loadings via a simple cocrystallization approach, yielding catalysts possessing well-dispersed Ga sites predominantly residing inside the pores and framework. Adjacency between Ga and BAS within the constraints of MFI channels makes these (Ga, Al)-H-MFI catalysts more active toward methane and propane activation and more selective toward aromatics compared to the Ga/MFI counterparts prepared by impregnation that inevitably leaves a large fraction of Ga at the external surface (i.e., without confinement and few adjacent BAS). Further, the effects of the Si/Al ratio on MPCA performance have been investigated for (Ga, Al)-H-MFI catalysts. Due to the multifold roles of BAS in the overall reaction sequence, an increased BAS concentration generally results in higher propane conversion and productivity of aromatics together with lower net methane conversion and severer coking.
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Journal of Materials Chemistry A
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2024
·
IF 10.7
Zhichao Ma,Chenyi Wang,Tianfang Yang,Gangya Wei,Jinrui Huang,Mengran Liu,Kun Zhang,Zunjie Zhang,Yang Liu,Shuyan Gao
Electrocatalytic nitrate (NO3−) reduction to ammonia (NH3) (NRA) is of great significance for solving the problem of urgent NO3− pollution in the environment and opening up a new route to synthesize NH3. However, NRA is limited by its multi-electron/proton transfer process and the NRA process relies heavily on atomic H* produced by H2O splitting, undergirding the necessity for effective NRA catalysts. Herein, three-dimensional (3D) porous phosphorus (P)-doped Cu–Ni alloy materials are constructed through a one-step electrodeposition synthesis. 3D porous materials modulate hydrophilicity and enrich active sites. The Cu d-band center can be tuned through Ni alloying to modify the adsorption energies of intermediates such as *NO3−, *NO2−, and *NH2. The hydrogenation evolution capacity of P promotes the hydrogenation process in the atomic H* path and effectively accelerates the NRA reaction rate. Density functional theory (DFT) calculations demonstrate that the charge transfer between the negatively charged Pδ− and the positively charged Niδ+ and Cuδ+ assists in generating more atomic H* for coupling with reaction intermediates, showing an enhanced catalytic activity at low overpotential. The optimal sample exhibits an exceptional NRA performance with an ammonia yield rate of 848.1 μmol h−1 cm−2 and a faradaic efficiency of 96.1%. This work provides a strategy for creating effective NRA catalysts through enhancing the atomic H* reduction strategy.
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