ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Lan-Ying Liu,Min-Hua Cui,John Justo Ambuchi,Shi-Ming Niu,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H* ads ) limit the applicability of this green process. In this study, bimetallic Pd–Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd–Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd 0 /Pd II ratio decreased by forming bimetallic Pd–Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd–Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H* ads production and tuning the reduction capability of H* ads . Noteably, the amounts and reduction potential of H* ads for Pd–Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H* ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H* ads .
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Lubricants
·
2024
·Vol. 12
·期 5
·163
·
IF 3.1
Yunqi Fang,Yang Sun,Fengqin Shang,Jing Zhang,Jiayu Yao,Zihan Yan,Hangyan Shen
Van der Waals heterostructures with incommensurate contact interfaces show excellent tribological performance, which provides solutions for the development of new solid lubricants. In this paper, a facile electrostatic layer-by-layer self-assembly (LBL) technique was proposed to prepare multi-layer van der Waals heterostructures tungsten disulfide/hexagonal boron nitride (vdWH WS2/h-BN). The h-BN and WS2were modified with poly (diallyldimethylammonium chloride) (PDDA) and sodium dodecyl benzene sulfonate (SDBS) to obtain the positively charged PDDA@h-BN and the negatively charged SDBS@WS2, respectively. When the mass ratio of PDDA to h-BN and SDBS to WS2were both 1:1 and the pH was 3, the zeta potential of PDDA@h-BN and SDBS@WS2were 60.0 mV and −50.1 mV, respectively. Under the electrostatic interaction, the PDDA@h-BN and SDBS@WS2attracted each other and stacked alternately along the (002) crystal plane forming the multi-layer (four-layer) vdWH WS2/h-BN. The addition of the multi-layer vdWH WS2/h-BN (1.0 wt%) to the base oil resulted in a significant reduction of 33.8% in the friction coefficient (0.104) and 16.8% in the wear rate (4.43 × 10−5mm3/(N·m)). The excellent tribological property of the multi-layer vdWH WS2/h-BN arose from the lattice mismatch (26.0%), a 15-fold higher interlayer slip possibility, and the formation of transfer film at the contact interface. This study provided an easily accessible method for the multi-layer vdWH with excellent tribological properties.
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RENEWABLE ENERGY
·
2024
·
IF 9
Huajing Zhou,Tiancheng Li,Fawen Zhang,Faze Chen,Zilian Liu,Rongrong Miao,Qingqing Guan,Lingxiang Zhao,Liang He
Intrinsic point defects in metal core-shell materials can regulate electron redistribution, thereby reducing catalytic energy barriers and enhancing their ORR activity. However, their specific contributions to electron transfer and mass transport pathways remain unclear. In this study, defect-rich hollow O Co @Co 3 O 4 nanoparticles were successfully synthesized using ZIF-67(Co) as a sacrificial template through controlled annealing and internal electric field substitution reactions. High-resolution electron microscopy analysis and density functional theory (DFT) calculations co-revealed the growth mechanism of Co and O vacancies, as well as antisite defects. The formation of oxygen vacancies significantly lowered the energy barrier for Co vacancy formation, playing a crucial bridging role in the development of antisite defects. The electric field polarization induced by Co-O atomic displacement resulted in asymmetric charge distribution, optimizing the adsorption of active hydrogen (H*) and oxygen atoms and facilitating the generation and release of reactive oxygen species (ROS). Electrocatalytic experiments demonstrated that under the combined action of singlet oxygen ( 1 O 2 ) and H*, bisphenol A (BPA) can be efficiently degraded. This study successfully bridges the knowledge gap between atomic defects and advanced electrocatalysis, providing a new perspective and insight for the in-depth analysis of the structure-performance relationship of electrocatalyst materials in the future.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Ling Ding,Lou Gao,Di Pan,Ke Du,Jiayu Yu,Wanyi Li,Yahong Zhang,Yi Tang
The utilization of racemic lactic acid (rac-LA) produced via chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (meso-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of meso-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L2A) in a one-step catalytic conversion of rac-LA to LD. Experimental results from various LA solutions with different L2A content indicate that the L2A content is critical for maximizing the selectivity of racemic lactide (D/L-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L2A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease meso-LD formation, and a LD yield of 60% with a D/L-LD/meso-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of D/L-LD and meso-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from rac-LA derived from chemical conversion.
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ChemistrySelect
·
2025
·Vol. 10
·期 7
·e202405464
·
IF 2
Kun Jia,Peng Jia
Graphical The asymmetric activation of anhydrous methanol molecules is realized by exogenous protons, the position and protonation position of asymmetric activation are determined, and the C─H bonding energy and reaction activation energy of some methanol molecules are reduced, and the asymmetric regulation of the non-oxidation dehydrogenation reaction process of anhydrous methanol molecules was realized. The activation of C─H bonds under mild conditions is a crucial step in the conversion of organic molecules. However, the simultaneous activation of C─H bonds in methanol can result in excessive oxidation, thereby diminishing the selectivity for formaldehyde production. We achieved selective activation of the C─H bonds in methanol under mild conditions by adjusting the proton concentration in an anhydrous methanol solution, which significantly enhanced the dehydrogenation rate of methanol. Additionally, we constructed related molecular models to identify the sites of asymmetric oxidation, providing new insights for further studies on C─H bond activation.
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ACS Catalysis
·
2024
·
IF 11.3
Zaixiang Xu,Fengcang Zhou,Hanchi Chen,Jianguo Wang
The regeneration of NAD(P)H and its analogues is crucial for biocatalytic processes. However, despite the efficiency of enzymatic catalysis in regenerating NAD(P)H, the sustainability of enzymes is often compromised, particularly under extreme catalytic conditions. Moreover, artificial cofactors may present advantages in certain reactions due to their stability and versatility, yet the substrate specificity of enzymes poses significant challenges to their regeneration through the enzymatic method. Therefore, it is imperative to develop a highly stable regeneration method that can be adapted to both natural and artificial cofactors. In this work, employing potassium-ion-doped carbon nitride (ionCN-0.2) as a catalyst not only achieves high-efficiency photocatalytic regeneration of NAD(P)H, comparable to that of glucose dehydrogenase (GDH), but also a remarkable ability to regenerate nicotinamide analogues. This enhanced performance stems from the tunable negative ζ-potential, which effectively adsorbs the positively charged [Cp*Rh(bpy)H2O]2+ mediator, resulting in enhanced regeneration kinetics of the nicotinamide moiety. The catalyst demonstrates superior performance compared to the reported systems; the optimal regeneration rate reaches 0.55 mmol L–1 gcat–1 min–1 and approaches enzymatic regeneration efficiency. Expanding the reaction conditions to a wider temperature and pH range also confirms the effectiveness and sufficient stability of this photocatalytic system, offering a promising strategy for stable cofactor regeneration in biocatalytic processes.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Zhiwei Zou,Hongxiang Zhang,Xuefeng Pan,Hui Shen,Jianying Yu,Tengfei Guo,Yonghao Wang
Electrocatalytic reduction of nitrate (NO 3 - ) to ammonium (NH 4 + ) is an environment friendly approach for treating nitrogen-containing wastewater. Consequently, electrocatalysts capable of effectively and selectively reducing NO 3 - to NH 4 + receives growing attention. However, Cu-based catalysts demonstrate limited efficiency and the drawback of generating toxic NO 2 - though it is prevalent in the field of electrocatalytic reduction of NO 3 - (NO 3 RR). In this work, a CuNi alloy was synthesized on a Co foil through electrodeposition (marked as CuNi@Co) and its electrocatalytic performance for NO 3 RR was evaluated. XRD, EDS mapping and XPS characterization indicate CuNi exists with alloy state. Electrocatalytic experiments demonstrate that CuNi@Co exhibits an exceptional FE NH3 of 99.12% at -0.64 V (vs. RHE). Importantly, no detrimental NO 2 - generated during NO 3 RR process because the reduction rate from NO 2 - to NH 4 + is faster than that from NO 3 - to NO 2 - . Mechanistic analysis suggests that Cu serves as a ‘reservoir’ to provide electrons to facilitate the reduction of NO 3 - to NO 2 - during NO 3 RR process and the synergistic effect of Ni and Cu promotes more active hydrogen (H*) to participate the reduction process of NO 2 - to NH 4 + not H 2 generation, ultimately improving FE NH3 . This work elucidates the role of electrons and H* in electrocatalytic nitrate reduction to ammonium for CuNi alloy, providing new insights into the reduction process of NO 3 RR for Cu-based materials.
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INTERNATIONAL JOURNAL OF FOOD SCIENCES AND NUTRITION
·
2019
·
IF 2.792
Yuanfeng Wu,Yuke Shen,Ye Zhu,Jothame Mupunga,Ligen Zou,Chao Liu,Shiwang Liu,Jianwei Mao
After consuming broccoli, isothiocyanates can be produced by the hydrolytic action of myrosinase from plant and/or microbiota. Using male C57BL/6 mice, the present study investigated the effects of broccoli ingestion on the myrosinase-like activity, NAD(P)H:quinone oxidoreductase 1 (NQO1) activity, diversity and composition of the gut microbiota. Compared with the control group, continuously feeding raw or hydrolysed broccoli increased the myrosinase-like activities of the colon and caecum contents, and also improved the NQO1 activity of the colon mucosa. Significant difference between the broccoli and control feeding groups were found. 16S rRNA gene sequencing indicated that broccoli ingestion profoundly affected the composition of the gut bacteria community. The correlation between the gut bacterial community composition and microbiota myrosinase-like activity was also studied. However, one type of glucosinolate, sinigrin, had no effect on these activities, indicating that broccoli component(s), other than glucosinolate, had increased the NQO1 and myrosinase-like activities.
研究领域:
营养学
·
微生物学
·
分子生物学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Yujia Xie,Fengyong Zhang,Pingle Liu,Fang Hao,Hean Luo
Direct functionalization of saturated C–H bonds by metalloporphyrin catalysts is among the topical and challenging areas within the chemical industry and synthetic chemistry. In this work, supported CoD(p-Cl)PPCl metalloporphyrin catalysts were prepared and characterized. It has been found that the CoD(p-Cl)PPCl/ZnO catalyst shows better catalytic activity than the supported catalyst (ZrO2, MCM-41, kaolin, Zr(OH)2, and boehmite (BM)) in cyclohexane oxidation with dioxygen. The effects of the reaction pressure, reaction temperature, and reaction time on the catalytic activity were considered by the supported CoD(p-Cl)PPCl/ZnO catalyst. The CoD(p-Cl)PPCl/ZnO catalyst can be facilely recovered and was recycled up to seven times without a significant decrease in catalytic performance. The average cyclohexane conversion and selectivity to KA oil are 10.98% and 84.34%, respectively, and the turnover number is 2.10 × 107.
研究领域:
催化化学
·
有机合成
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工业化学
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材料化学
·
绿色化学
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Lu Wang,Hong Li,Yue Dai,Erzhu Sun
Dopamine (DA) can self-polymerize to form polydopamine (PDA) under weak alkaline conditions in the presence of oxygen, creating vibrant structures at the gas–liquid interface. However, the issue of the polydopamine film cracking and easily peeling off from the fabric surface remains unresolved. In this article, we report the rapid polymerization of dopamine in a CuSO 4 /H 2 O 2 system, resulting in the preparation of polydopamine-structured colored cotton fabrics through the stepwise addition of 3-aminopropyltriethoxysilane (KH550) and polyethyleneimine (PEI). Structured color cotton fabrics were hydrophobically treated by a simple impregnation technique using the hydrophobic agent cetyltrimethoxysilane (HDTMS). This improvement suggests that the covalent bonding of PEI with PDA, along with its assembly on the fabric surface, enhanced the homogeneity and continuity of the structural color film, resulting in a brighter and more uniform fabric surface color. After HDTMS treatment, the structural color film on PDA/KH550/PEI-Cotton was converted from a hydrophilic to a hydrophobic state, with a static water contact angle averaging approximately 152.375°. The hydrophobic treatment provided the structural color fabrics with good film stability and resistance to washing, while their surface coloration remained largely unaffected. This method provides a new research idea for eco-dyeing of cotton fabrics.
研究领域:
材料科学
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纺织功能材料
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表面化学
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纳米结构色
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绿色染整技术
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Jianning Zhang,Yanpei Dang,Tianhao Li,Yangzhong Zhao,Liantai Duan,Ke Chen,Xiao Zhang,Hengli Duan,Wensheng Yan,Sihua Feng,Gang Shao,Zhaoju Yu,Qing Huang,Yujie Song
Silicon boron carbonitride (SiBCN) ceramics have garnered significant attention due to their exceptional high-temperature stability, resistance to creep, and favorable electrical properties. However, the ceramicization mechanism of covalently bonded boron atoms in polyborosilazane (PBSN), which is crucial in determining the structural and crystalline phase evolution of silicon boron carbonitride (SiBCN) ceramics through the polymer-to-ceramic process, still needs further clarification for the design of advanced ceramics. Therefore, PBSN precursors constructed with B–C bonds were systematically investigated in the polymer-to-ceramic conversion process. B–C bonds were transformed into B-N bonds between 300°C and 600°C, ultimately resulting in the formation of h-BN at high temperatures. Meanwhile, higher levels (8.11–14.12%) of B facilitated the formation of SiC at equivalent temperatures but hindered the formation of Si 3 N 4 crystal nuclei. That is due to the formation of B–N and NB 3 units, which inhibited the formation of Si–N bonds and SiN 4 units, thereby interfering with the nucleation process of Si 3 N 4 and facilitating the crystallization of SiC. This study offers valuable insights for regulating the microphase evolution and properties of PDC nanocomposites.
研究领域:
材料科学
·
陶瓷材料
·
聚合物衍生陶瓷
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固态化学
·
高温材料
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Small Methods
·
2026
·
IF 8.7
Xiaochen Feng,Zihao Huang,Mingwei Fang,Meiling Wang,Jinyue Ma,Zewen Wang,Ying Zhu,Lei Jiang
Electrochemical CO 2 reduction (CO 2 RR) to ethanol offers a sustainable route for carbon utilization and energy storage, yet achieving high ethanol selectivity under limited CO 2 availability remains a significant challenge. The central issue is the lack of quantitative understanding of how the interfacial * CO and * H intermediates jointly govern product selectivity. Here, we establish an interfacial coverage regulation strategy by embedding Cu nanoparticles into an imine-functionalized covalent organic framework (Cu/Im-COF). The imine-rich interface enriches CO 2 adsorption while modulating proton transfer, enabling a balanced surface coverage of * CO and * H, identified as the key selectivity descriptor ( θ *CO/*H ) for ethanol formation. Operando Raman spectroscopy, density functional theory calculations, confirms that an optimized θ *CO/*H stabilizes the * HCCHOH intermediate and lowers its formation barrier. Quantitative integration of Raman features allows direct determination of θ *CO/*H , revealing a volcano-type dependence of ethanol selectivity on this descriptor. A maximum ethanol Faradaic efficiency of 56% is achieved at log( θ *CO/*H ) ≈ 3.0, a current density of 700 mA cm − 2 , and a 15% CO 2 feed. This work establishes θ *CO/*H as a quantitative bridge between intermediate coverage and reaction kinetics, providing a mechanistic framework for rational design of CO 2 RR catalysts with high ethanol selectivity under CO 2 -constrained conditions.
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