SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Faxun Wang,Junyi Lin,Yuxuan Huang,Jiguang Zhao,Bing Tian,Liang Zhao,Bofeng Luo,Zhenliang Ye,Hao Yang,Guotao Duan
Reliable, drift-resistant monitoring of SF 6 enrichment in air near gas-insulated switchgear (GIS) leak points remains challenging for compact and low-cost sensing nodes. Here we report a thermal-conductivity-differential sensor enabled by a materials-circuit co-design: a hierarchical AlN@h-BN/MWCNT nanocomposite coating is integrated onto a Pt-coil element and read out by a Wheatstone bridge with a sealed reference arm and differential amplification. The ternary architecture exhibits a well-developed mesoporous framework with a high BET surface area (111.03 m 2 ·g −1 ), promoting efficient gas transport within the sensing layer and strengthening the thermal-conductivity-induced perturbation of the bridge balance. Under synthetic dry air (21% O 2 /79% N 2 ) at 25 ± 1℃, the output is monotonic over 0.1–5.0% SF 6 , with a recommended linear regime of 0.1–1.0% for quantitative readout; the baseline noise (σ air = 0.16 mV) yields an estimated LOD (3σ) of 0.0654% (∼654 ppm), while 0.1% is the lowest experimentally validated concentration. The optimized excitation voltage (3.0 V) maximizes response by balancing gas-phase modulation against increased non-gaseous heat losses at higher temperatures. The sensor shows reversible cycling (52/23 s response/recovery), humidity-tolerant operation (± 8% deviation over 20–80% RH), and < 5% degradation over 90 days; as expected for a TCD-type mechanism, cross-responses are governed by thermal conductivity rather than chemical selectivity.
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高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ying Zhang,Bin Wei,Hao Liang
An organometallic complex-catalyzed artificial coenzyme regeneration system has attracted widespread attention. However, the combined use of organometallic complex catalysts and natural enzymes easily results in mutual inactivation. Herein, we establish a rhodium-based metal–organic framework (MOF)-on-MOF difunctional core–shell nanoreactor as an artificial enzymatic NAD(P)H regeneration system. UiO67 as the core is used to capture rhodium molecules for catalyzing NAD(P)H regeneration. UiO66 as the shell is used to specifically immobilize His-tagged lactate dehydrogenase (LDH) and serve as a protection shield for LDH and [Cp*Rh(bpy)Cl]+ to prevent mutual inactivation. A variety of results indicate that UiO67@Rh@UiO66 has good activity in realizing NAD(P)H regeneration. Noteworthily, UiO67@Rh@UiO66@LDH maintains a high activity level even after 10 cycles. This work reports a novel NAD(P)H regeneration platform to open up a new avenue for constructing chemoenzyme coupling systems.
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PubMed
高影响因子
ICARUS
·
2022
·
IF 3.657
A. García Muñoz
Photoelectrons , the fast electrons produced in the photoionization of planetary atmospheres , drive transformations in the atmospheric gas that are often inhibited by energy considerations for thermal electrons. The transformations include excitation and ionization of atoms and molecules, which affect the detectability of these gases and constrain the fraction of incident stellar radiation that transforms into heat. To gain insight into these important questions, we build a Monte Carlo model that solves the slowing down of photoelectrons in a gas with arbitrary amounts of H and He atoms and thermal electrons. Our novel multi-score scheme differs from similar tools in that it efficiently handles rare collisional channels, as in the case of low-abundance excited atoms that undergo superelastic and inelastic collisions . The model is validated and its performance demonstrated. Further, we investigate whether photoelectrons might affect the population of the excited hydrogen H(2) detected at some exoplanet atmospheres by transmission spectroscopy in the H- α line. For the ultra-hot Jupiter HAT-P-32b, we find that photoelectron-driven excitation of H(2) is inefficient at the pressures probed by the line core but becomes significant (yet sub-dominant) deeper in the atmosphere where the line wings form. The contribution of photoelectrons to the destruction of H(2) either by collisional deexcitation or ionization is entirely negligible, a conclusion likely to hold for exoplanet atmospheres at large. Importantly, photoelectrons dominate the gas ionization at the altitudes probed by the H- α line, a fact that will likely affect, even if indirectly, the population of H(2) and other tracers such as metastable helium. Future modeling of these excited levels should incorporate photoelectron-driven ionization.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xixi Chen,Wanyi Fu,Yulong Yang,Yanjun Li,Kai Yang,Xuanbo Xu,Xihui Zhang
Atomic H* has been reported to be thermodynamically feasible for activating hydrogen peroxide (H 2 O 2 ) to produce radicals, while the nonradical pathway and the contributions of metal sites and atomic H* in H 2 O 2 activation need further exploration. In this study, a TiO 2 @MnO 2 catalyst was synthesized via a facile hydrothermal method and surprisingly found to produce atomic H* over Mn sites in water without external energy input (e.g., light and electricity). Atomic H* plays an essential role in the activation of H 2 O 2 via a nonradical pathway, which induces the removal of tiamulin up to 80.4–91.7% in 20 min at a wide pH range of 4.0–11.0. Density function theory calculations prove that atomic H* owns a much lower total energy barrier (ΔG total = 0.68 eV) for the decomposition of H 2 O 2 to generate superoxide and singlet oxygen than Mn sites (ΔG total = 2.90 eV). This study is a re-visit to the mechanism of activating H 2 O 2 via atomic H* for efficient degradation of emerging organic contaminants .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tian-Yu Liu,Cong Wang,Yong-Zhe Han,Chang Bai,Hai-Tao Ren,Yong Liu,Xu Han
Bi 2+x WO 6 are a group of reactive photocatalysts in the photooxidation of various contaminants. However, their catalytic reactivity in the persulfate (PS)-based oxidation processes in the absence of light is still unknown. In this study, Bi 2.15 WO 6 shows a high reactivity in the catalytic oxidation of bisphenol A (BPA) by PS in the absence of light under alkaline conditions, and 20 mg L -1 BPA can be rapidly removed within 30 min at pH 10.0 with the low stoichiometry ratio of 1.79 between consumed PS and removed BPA. Characterizations of the oxidation products indicate that 98.4% of soluble BPA has been oxidatively polymerized to BPA polymers, instead of being oxidized to CO 2 and H 2 O. FTIR, Raman, XPS and electrochemical analyses confirm that surface Bi(III) is the reactive site for the adsorption of BPA and PS, which then initiates reactions between BPA and PS. DFT calculations reveal that the O-O bond in PS is moderately activated via the nonradical pathway after adsorbing on Bi(III), instead of being decomposed to SO 4 •− , followed by H-abstraction from BPA by the activated PS with the formation of phenoxyl radicals and the subsequent polymerization to BPA polymers. The apparently lower energy barrier from adsorbed BPA (Δ G = 0.056 eV) than that from dissolved BPA (Δ G = 0.263 eV) further reveals that H-abstraction from adsorbed BPA to the activated PS on the surface of Bi 2.15 WO 6 is more favorable than that from dissolved BPA. This study gives new insight on the efficient removal of recalcitrant contaminants via the H-abstraction pathway.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 20
·6268-6284
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IF 6.177
Tingyu Liang,Jialing Chen,Sen Wang,Pengfei Wang,Zhangfeng Qin,Fang Jin,Mei Dong,Jianguo Wang,Weibin Fan
A series of H-MCM-22 zeolites with different Si/Al ratios (H-M22-x, x = 15–90) were hydrothermally synthesized by boron incorporation to investigate the influences of acid density on the methanol-to-hydrocarbon (MTH) performances and deactivation behaviors. The acid density of H-M22-x zeolites is nearly proportional to their aluminum contents; the residual boron barely affects the overall acidity of H-M22-x zeolites. 27Al and 29Si MAS NMR experiments support the existence of competitive occupancy of various framework T sites among boron, aluminum and silicon during zeolite synthesis, which leads to different distribution of Brønsted acid sites/framework aluminum among three types of pores in H-MCM-22 zeolites. Increasing the Si/Al ratio of H-M22-x zeolites leads to a gradual increase in the proportion of Brønsted acid sites in supercages while those in sinusoidal channels decrease. However, the acid density has a significantly larger impact than acid distribution on the MTH performances of H-M22-x zeolites. Increasing the acid density can accelerate the hydrogen transfer reactions in the MTH conversion and promote the formation of aromatics, ethene, and alkanes. The deactivation of H-M22-x zeolites with low acid density (x = 50–90) is mainly ascribed to coke covering the acid sites inside the micropores and partly blocking the pore mouths. Nevertheless, the deactivation of H-M22-x zeolites with high acid density (x = 15–30) is mainly caused by massive coke deposition on the external surface which blocks the pore mouths of inner micropores. The coke on the external surface exhibits a lower decomposition temperature than that inside the micropores. The deactivation behaviors of H-M22-x zeolites for the MTH reaction can be divided into three stages. Firstly, rapid deactivation of supercages occurred for all the H-M22-x zeolites in spite of their different acid densities, suggesting a much stronger influence of pore structure than acidity on the initial deactivation behaviors of H-M22-x zeolites. Secondly, the acid sites in sinusoidal channels of H-M22-x zeolites are highly resistant to coke formation, which dominates the MTH reaction in the second stage. Finally, with the continuous formation of coke in the surface pockets, which gradually covers the acid sites and pore mouths of sinusoidal channels, complete deactivation of H-M22-x zeolites can be observed. GC-MS and UV-vis analysis of partly or completely deactivated H-M22-x zeolites reveals that the retained species in H-M22-x zeolites gradually condense into bulky hydrocarbon species through successive hydrogen transfer reactions and form methylbenzenes, naphthalene, polymethylnaphthalenes, phenalenone, pyrenes and eventually graphite-like carbonaceous species.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Junqiao Jiang,Zhen Li,Min Xiao,Shuanjin Wang,Kenji Miyatake,Yuezhong Meng
Phosphoric acid (PA)-doped polymer electrolyte membranes are the most promising materials for high-temperature proton exchange membranes (HT-PEMs). However, their development is subject to the compromise between proton conductivity and phosphoric acid (PA) doping level. Here, an ether-free QPAF-4 membrane (a copolymer containing perfluoroalkylene and fluorenyl groups with pendant ammonium groups) is directly doped with phosphoric acid and studied as HT-PEMs. Due to the intrinsic micro-phase separation structure of QPAF-4 matrix and strong interaction of quaternary ammonium (QA)-PA, the PA-doped membranes possess high proton conductivity and eminent PA retention at comparatively low PA doping level, respectively. The QPAF-4 membrane with 150% PA uptake (QPAF-4-150%PA) offers a proton conductivity of 52 mS cm −1 at 160 °C. As expected, the single cell with QPAF-4-150%PA membrane shows the maximum peak power density of 683 mW cm −2 at 160 °C under anhydrous condition. Meanwhile, the single cell exhibits excellent durability over a period of 60 h with only a slight reduction in voltage of 3.1%. These results indicate that the as-prepared PA-doped quaternized polymer with micro-phase separation structure seems to offer a promising way to develop performing and long-life HT-PEMs with low PA doping levels.
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高影响因子
Solar RRL
·
2021
·Vol. 5
·期 12
·2100559
·
IF 8.582
Hong-Hong Zhang,Zi-Chun Zhou,Yu-Jie Dong,Li Zhang,Hong-Yan Chen,Dai-Bin Kuang
Utilizing halide perovskites for photocatalytic aromatic C( sp 3 ) H bond activation remains a great challenge due to the serious recombination of photogenerated charge carriers and slow reaction dynamics of the materials themselves. Herein, a lead-free perovskite-based hybrid of Cs 3 Sb 2 Br 9 /g-C 3 N 4 nanosheet is constructed and applied for photocatalytic aromatic C( sp 3 ) H bond activation, which shows enhanced photocatalytic performance. By introducing ultrathin g-C 3 N 4 nanosheets as the heterogeneous nucleation sites, size-reduced and well-dispersed Cs 3 Sb 2 Br 9 nanocrystals can be obtained. The as-formed close contact and high-quality heterointerface between Cs 3 Sb 2 Br 9 and g-C 3 N 4 provides pathways for fast charge transfer which is beneficial to improve the separation efficiency of photogenerated electron−hole pairs. Under visible light irradiation, the Cs 3 Sb 2 Br 9 /g-C 3 N 4 hybrid photocatalyst can effectively oxidize toluene toward benzaldehyde and benzyl alcohol with a total conversion rate of 8346.8 μmol g −1 h −1 , which is 26.6- and 6.0-fold that of pure g-C 3 N 4 and Cs 3 Sb 2 Br 9 , respectively. This work demonstrates the potential of all-inorganic lead-free halide perovskite-based heterostructures for photocatalytic organic reactions.
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高影响因子
Additive Manufacturing
·
2021
·
IF 10.998
Yuchao Wu,Mingen Fei,Tingting Chen,Chao Li,Tengfei Fu,Renhui Qiu,Wendi Liu
Thermoplastic elastomers exhibit high softness, stretchability, recoverability, and reprocessibility, but their manufacture requires high cost and long processing time. Photocuring 3D printing is a remedial processing method as it enables rapid fabrication at room temperature. However, it is difficult to print thermoplastic elastomers by photocuring 3D printing because the generated linear polymers easily dissolve in liquid precursors during printing. Herein, stretchable, self-healing, and renewable palm oil (PO)-based elastomers were prepared from UV-responsive vinyl PO monomers via photocuring 3D printing. Fast solid-liquid separation was achieved via hydrogen bonds and Zn 2+ -ligand coordination (non-covalent crosslinking) to slow down the dissolution of crosslinked polymers in the monomer liquid . The non-covalent bonds endowed the elastomers with high tensile strength (~4.2 MPa) and elongation at break (~851%). Additionally, the elastomers are mainly prepared from biobased, renewable, and low-cost PO feedstocks . Most importantly, the dual dynamic crosslinked network resulted in superior stress relaxation, shape programming, and self-healing behavior of the elastomers. The method described may enhance the application scope of thermoplastic elastomers and 3D printing.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Xiao Zhao,Xuan Shi,Zhongshun Chen,Long Xu,Chengyi Dai,Yazhou Zhang,Xinwen Guo,Dongyuan Yang,Xiaoxun Ma
A series of ZnO-ZrO 2 solid solutions with different Zn contents were synthesized by the urea co-precipitation method, which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts. As a new benzene alkylation reagent, syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene. A suitable ratio of ZnO-ZrO 2 led to the significant improvement in the catalytic performance, and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C 9 + aromatics. The highest benzene conversion of 89.2% and toluene/xylene selectivity of 88.7% were achieved over 10% ZnO-ZrO 2 &H-ZSM-5 (Si/Al = 23) at a pressure of 3 MPa and a temperature of 450 °C. In addition, the effect of the zeolite framework structure on product distribution was examined. Similar to the molecular dynamics of aromatic hydrocarbons , H-ZSM-5 zeolites comprise 10-membered-ring pores, which are beneficial to the activation of benzene; hence, the conversion of benzene is higher. H-ZSM-35 and H-MOR zeolites exhibited small eight-membered-ring channels, which were not conducive to the passage of benzene; hence, the by-product ethylbenzene exhibits a higher selectivity. The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance, and the powder mixing method was more conducive to the conversion of syngas and benzene.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Xiao-Lu Sun,Zan Liu,Zhi-Lin Cheng
The Cu-intercalated layered h-BN/N-doped carbon-nanofiber composite films (PAN-Cu/ABN-CNFs) were successfully prepared by the combination of the electrospinning technique and the one-pot carbonization process, using the mixed solution of polyacrylonitrile (PAN) and Cu-intercalated activated boron nitride (Cu/ABN) as carbon precursor. A series of characterizations proved that the PAN-Cu/ABN-CNFs possessed the distinguished merits in the structure and composition, such as the pore feature of the micropore (0.076 cm 3 /g)-mesoporous (0.3582 cm 3 /g) structure, the structure of the exfoliated h-BN nanosheets , the low-coordination high-content N (11.65 at%) and the existence of self-reducing Cu nanoparticles (0.5 at%). For adapting the actual application, the mechanical properties of the PAN-Cu/ABN-CNFs were comprehensively evaluated, showing that the PAN-Cu/ABN-CNFs films had the robust tensile strength and bending properties as well as the desirable wear resistance. Furthermore, the selective adsorption desulphurization of the PAN-Cu/ABN-CNFs were examined by the selective adsorption removal of thiophene (TH) from the simulated oil, indicating that the optimum adsorption capacity of the fresh films was up to 78.38 mg/g in 800 mg/L initial concentration and the adsorption capacity after the four-time regeneration recycling still approached 74.894 mg/g. Finally, the adsorption kinetics , isotherm and thermodynamic studies suggested that the adsorption behavior of TH over the PAN-Cu/ABN-CNFs should be better described by the correlation coefficients of Avrami fractional-order kinetics and Liu isotherm, while the thermodynamic studies showed a favorable exothermic and spontaneous adsorption mechanism.
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高影响因子
APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Xinyu Li,Shunyu Han,Dongdong Guan,Nanzhe Jiang,Jingzhe Xu,Sang-Eon Park
The direct synthesis of H-ZSM-5 catalysts from natural aluminosilicate clays is important for the conversion of raw clay resources to high-value-added products. Herein, the solid-like-state conversion was used to directly prepare nano-H-ZSM-5 with uniform morphology and particle size (~300 nm) from leached illite (ISR) as both Si and Al source. Crystallization kinetics indicated that the reactivity of ISR is similar to that of commercially fabricated products and ISR could be rapidly (within 5 h) converted into nano-H-ZSM-5, the crystallinity , morphology, and crystal size of which were strongly affected by the amount of tetrapropylammonium hydroxide (TPAOH). Additionally, the residual Al of ISR uniformly intruded the H-ZSM-5 framework to provide active sites for the methanol-to-aromatics reaction. The catalytic performance stability and BTX selectivity of nano-H-ZSM-5 for this reaction surpassed those of a commercial ZSM-5 catalyst because of the synergistic effect among the specific surface area and volume of micropores , uniform morphology and particle size, and homogeneously distributed acidic sites. This rapid, efficient, and cleaner synthesis reported herein was shown to have no necessity of ion exchange with ammonium salts, to be H-form of ZSM-5 as well as improve the productivity of HZSM-5 catalysts. And consequently, it is expected to reduce the cost of synthesis and provide an opportunity for the comprehensive development and utilization of illite clay resources.
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高影响因子
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