Surfaces and Interfaces
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2024
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IF 5.7
Yufeng Xiong,Yingjiang Li,Zhengfei Hu,Zhengquan Sun,Yiliang Chen,Yang Zhang,Lijie Dong
Fabricating electrodes simultaneously possessing remarkable flexibility, excellent mechanical properties, and high energy density remains a significant challenge in flexible lithium-ion batteries (LIBs). Herein, a series of flexible organic composite films were prepared with high-loading polytriphenylamine (PTPA) and the derivative (PTPA-PO) as active material, along with carbon nanotubes (CNTs) serving as conductive filler. The fabrication employed the polyethylene oxide (PEO) assisted nonsolvent (or poor solvent) induced phase separation electrospinning (NIPSE) method. Subsequently, the fiber morphology and electrochemical applications of the flexible organic composite films were systematically studied. Notably, the 60 % PTPA-PO/20 % CNTs/PEO flexible electrode with a high-loading active material of 60 wt% exhibits a significant discharge capacity of 146.6 mAh·g −1 and a favorable discharge platform ∼ 3.7 V vs. Li. Furthermore, the inherent flexibility of electrode contributes to efficient and stable transport of ions and electrons, resulting in a fine capacity retention of 93.3 % after 100 cycles. The improvement of electrochemical performance can be rationalized by the unique internal conductive network and crater-like surface structure of the fibers formed through the NIPSE method. This work provides an efficient method to fundamentally improve the energy storage performance and flexibility of LIBs.
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Journal of Energy Chemistry
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2025
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IF 14.9
Weixin Miao,Songliang Liu,Yuewen Sun,Cong Zhang,Meixiang Zheng,Guangshuo Li,Xuejing Cui,Xin Zhou,Luhua Jiang
Electrocatalysis, a form of heterogeneous catalysis, is closely associated with both catalyst properties and the catalyst/electrolyte interfacial microenvironment. Herein, we rationally design and synthesize a unique PdCu nano-sea urchins (PdCu NSUs) featured with high-curvature nanotips, by which the interfacial microenvironment is expected to be tailored to the electrocatalytic reactions. PdCu NSUs exhibit excellent activity for ethanol electrooxidation, with a specific activity of 4.11 mA cm −2 and a mass activity of 2.24 mA μg Pd −1 , and a high Faraday efficiency (FE) of 96.4% toward acetic acid. COMSOL finite element simulations confirm that the unique nanotips could induce a local electric field due to the accumulation of positive charges in the nanotips, resulting in enrichment of OH - at the catalyst surface to promote the formation of Pd−OH ads , a species required by ethanol dehydrogenation. Furthermore, DFT calculations and in-situ electrochemical Fourier transform infrared spectroscopy discover that the d-band center of Pd significantly downshifts in PdCu alloy, which facilitates the desorption of the produced acetic acid. This work provides a new electrocatalytic material with high-curvature nanotips, and also clarifies how the material morphology, by inducing local electric fields, affects the interfacial microenvironment and thus the catalytic activity and selectivity.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jiuli Chang,Lili Wang,Zhanqiang Hu,Songsong Zhi,Dapeng Wu,Kai Jiang,Zhiyong Gao
Selective ethylene glycol oxidation reaction (EGOR) to specific C2 species offers a promising approach to pair with cathodic hydrogen evolution reaction (HER) for electrochemical upcycling of waste polyethylene terephthalate (PET) plastic into high-value chemicals and H 2 . Efficient catalyst with tailored adsorptive interaction strength with intermediates is pivotal to fulfill such a scenario. Herein, a self-supported PdNi/NF electrode with deposition of PdNi hybrid onto nickel foam (NF) substrate was prepared by a gentle replacement reaction, which demonstrated high catalytic activity for EGOR toward glycolate with high faradaic efficiency (90 ± 2 %), decent yield (0.7 ± 0.01 mmol h −1 cm −2 ) and acceptable stability at a low applied potential of 0.8 V, which enabled electrosynthesis of glycolate via electrooxidation of PET hydrolysate. Meanwhile, a self-supported Cu, Co bimetallic phosphide onto NF substrate (CuCoP/NF) was prepared for HER catalysis, which featured a low overpotential of 117 mV at cathodic current density ( J ) of −100 mA cm −2 and decent durability. The further pairing of anodic EGOR and cathodic HER enabled electrolysis of PET hydrolysate to coproduce glycolate and H 2 at an energy-saving manner. This work provides a viable paradigm for coproduction of glycolate and H 2 from electrochemical upcycling of PET plastic, and presents essential instruction for reclamation of obsolete resource via sustainable and waste-to-treasure manner.
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ARCHIVES OF BIOCHEMISTRY AND BIOPHYSICS
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2025
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IF 3
Yilu Sun,Jia Zhao,Jianhui Rong
Skin hyperpigmentation due to UV-induced tyrosinase activation and melanin overproduction is an ongoing challenge in cosmetic and dermatological applications. While resveratrol analogues show anti-melanogenic potential, the structure-activity relationships of their glycosylated derivatives remain underexplored. Here, we investigate how the vinyl moiety in the food-derived stilbenoid glycoside piceid (resveratrol-3- O -β-glucoside) affects tyrosinase inhibition. We reduced the vinyl moiety to yield dihydropiceid by catalytic hydrogenation and systematically assessed both compounds for anti-melanogenic effects. As results, piceid exhibited superior monophenolase inhibition over dihydropiceid in enzyme kinetics, while both compounds showed comparable diphenolase inhibition. Cellular assays revealed that piceid reduced melanin production by 59.2 % at 25 μM in α-MSH-stimulated B16F10 melanoma cells, whereas dihydropiceid showed weaker activity (<25 % reduction). MolgpKa analysis indicated that the vinyl moiety lowered the 4′-OH pKa (9.7 vs. 9.9), while UV–vis spectroscopy validated that the vinyl moiety enhanced the copper chelation capacity of piceid (ΔOD: 0.459) over dihydropiceid (ΔOD: 0.233). Molecular docking revealed that 4′-OH in piceid closely coordinated the tyrosinase binuclear copper center, whereas molecular dynamics simulation validated that hydrogen bonding supports the binding of both compounds to tyrosinase. Collectively, this study establishes the vinyl moiety in dietary stilbenoids as a critical pharmacophore for tyrosinase inhibition and thereby provides a molecular basis for developing natural anti-hyperpigmentation functional foods or cosmeceuticals.
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Advanced Science
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2025
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IF 14.1
Yanyan Yu,Yilin Li,Yuhan Lou,Mengyuan Chen,Yongzhuang Liu,Haipeng Yu
Catalytic refining of lignin holds promise for producing sustainable platform chemicals. In this work, a gaseous hydrogen-free catalytic hydrodeoxygenation system is developed for upgrading lignin-derived phenols to alkane chemicals. Commercially available Raney Ni and HZSM-5 are used as a combinational catalyst, with isopropanol serving as the hydrogen-donating solvent. By modifying the temperature and the ratio of Raney Ni to HZSM-5, the reaction pathways for hydrogenation and deoxygenation can be tailored to specific requirements. As a result, a 97.1% yield of alkane fuels is achieved, with 64.4% propylcyclohexane and 32.7% propylbenzene obtained in one-pot reaction from the hydrodeoxygenation of 2-methoxy-4-propylphenol using a 3:1 mass ratio of Ni to HZSM-5, further increasing the ratio of HZSM-5 leads to a selectively production of propylbenzene in 62.0% yield. Through careful regulation of the catalytic system and the design of hydrogenation–deoxygenation pathways, excellent yields of 4-propylcyclohexanol (92.2%), propylcyclohexene (93.3%), and propylcyclohexane (93.2%) are directionally achieved. The catalyst maintained a conversion rate of over 99% after five cycles, demonstrating excellent robustness. This study offers a strategic system that expedites the selective upgrading of lignin-derived chemicals, heralding a pathway toward sustainable fuels and chemicals.
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CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Xueting Zhao,Qingqing Qiu,Jinshan Sun,Xinhao Cheng,Lifen Liu,Jiefeng Pan
Nanofiltration (NF) membrane technology serves as an efficient method for separation and purification, playing a vital role in various industrial fields such as water treatment, food processing, and pharmaceutical manufacturing. However, there are still drawbacks, such as limited flux due to densely crosslinked composite layer and poor stability in solvents. In this study, we report the fabrication of the thin-film composite (TFC) NF membrane using Tröger’s base-derived building block, aiming to manipulate intrinsic pore structures of the as-synthesized ultra-thin composite layer by introducing rigid dihedral units. The interfacial polymerization process is employed to enable the polycondensation of Tröger’s base-based diamine monomer and tri-aldehyde monomer via Schiff base reaction. The effects of monomer concentration, immersion time, interfacial polymerization reaction time, heat treatment time and temperature on the performance of NF membrane were studied. The optimized NF membrane presents a rejection of Methyl blue (MB) above 95.3 % and achieves a high water permeance of 43.4 L·m −2 ·h −1 ·bar −1 . The water permeance is 2–3 times higher than the reported NF membranes with similar rejection ability. In addition, Tröger’s base-derived TFC NF membrane exhibits excellent long-term stability and good organic solvent tolerance. Considering the high water permeance and separation efficiency, the present membrane has significance in dye removal and separation processes.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qianlin Ju,Tao Chen,Qianhui Xie,Manli Wang,Kaige Zhao,Tong Liu,Liang Fu,Haozhi Wang,Zelin Chen,Changjiu Li,Yida Deng
As a novel electrochemical energy conversion device, direct ethanol fuel cells are currently encountering two significant challenges: CO poisoning and the difficulty of C–C bond cleavage in ethanol. In this work, an amorphous PdS nanowires/ultrafine IrMnOx bimetallic oxides (denoted as a-PdS/IrMnOx NWs) catalyst with abundant oxide/metal (crystalline/amorphous) inverse heterogeneous interfaces was synthesized via a hydrothermal process succeeded by a nonthermal air-plasma treatment. This unique interfacial electronic structure along with the incorporation of oxyphilic metal has resulted in a significant enhancement in the electrocatalytic performance of a-PdS/IrMnOx NWs toward the ethanol oxidation reaction, achieving current densities of 12.45 mA·cm–2 and 3.68 A·mgPd–1. Moreover, the C1 pathway selectivity for ethanol oxidation has been elevated to 47%, exceeding that of other as-prepared Pd-based counterparts and commercial Pd/C catalysts. Density functional theory calculations have validated the findings that the decoration of IrMn species onto the amorphous PdS surface has induced a charge redistribution in the interface region. The redistribution of surface charges on the a-PdS/IrMnOx NWs catalyst results in a significant decrease in the activation energy required for C–C bond cleavage and a notable weakening of the CO binding strength at the Pd active sites. Consequently, it enhanced both the EOR C1 pathway selectivity and CO poisoning resistance to the a-PdS/IrMnOx NWs catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Xinyu Gu,Huiyu Sun,Nannan Zhang,Jun Yu,Jie Li,Changqing Ye,Yukou Du
One-dimensional (1D) Pd-based nanowire materials, characterized by high aspect ratios and exposed high-index crystal surfaces, are widely developed in the field of direct fuel cells. However, their synthesis methods are often not universal and necessitate demanding conditions, including high temperatures and metal templates, leading to resource consumption. In this study, we present a simple and universal one-step method for synthesizing PdM (Sb, Ir, and Bi) nanowire networks (NNWs) at room temperature. Leveraging their structural advantages and the synergistic effects between bimetals, PdM NNWs demonstrate exceptional electrocatalytic performance, exhibiting higher mass and specific activities as well as enhanced durability compared to Pd/C for the ethylene glycol and glycerol oxidation reactions. Notably, PdSb NNWs excelled in electrochemical tests, achieving the highest mass activities of 7.55 and 5.59 A mg −1 for the ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR), respectively. Additionally, due to the semi-metallic properties of Sb, which can flexibly modify the chemical environment of Pd, the PdSb NNWs exhibited superior antitoxicity and a significantly lower decay of current density across three consecutive chronoamperometry (CA) tests. This research advances the synthesis of palladium-based nanostructures, providing impetus for the design of highly efficient electrocatalysts in the realm of direct alcohol fuel cells.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Feng Feng,Jiaying Zhang,Lu Yu,Haixin Wang,Heda Ding,Jifan Cheng,Miaolan Wang,Fangfang Chen,Jiahui Zhang,Lingling Guo,Chunshan Lu,Qunfeng Zhang,Xiaonian Li
In order to develop an efficient and environmentally friendly method for the recovery of precious metals, a functionalized ionic liquid containing free radicals (1-methyl-3-(2-oxo-2-(2,2,6,6-tetramethyl-1-oxo-4-piperidinoxy) butyl) imidazole trichloro-1-bromoaluminium salt) was designed and synthesized. This was achieved by combining 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), which possesses oxidizing properties, with halide ions that exhibit complexing abilities. Notably, under optimal conditions, a maximum gold dissolution rate of 100 % was attained. X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and Raman spectroscopy analyses were conducted to elucidate the dissolution mechanism. Ultimately, these functionalized ionic liquids can be utilized for the dissolution of precious metals in CPU pins and waste catalysts. This study presents an effective approach for the recovery of precious metals.
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BIOMASS & BIOENERGY
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2024
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IF 5.8
Zhenjing Jiang,Wuyu Wang,Xuelai Zhao,Xinghua Zhang,Qi Zhang,Longlong Ma
Production of jet fuel is not only promising but challenging in the field of biomass utilization. Here we proposed a novel route to produce highly branched alkanes with ultra-low freezing point using n-butyraldehyde as feedstock by self-aldol condensation and subsequent hydrodeoxygenation (HDO). The catalyst characterization revealed that the MgO-SiO 2 catalyst played an acid-base synergetic effect role in the self-aldol condensation of n-butyraldehyde using n-butanol as solvent, which obtained C8 oxygenate and C12 oxygenate with yield of 69.3 % and 26.8 % respectively. The medium Brønsted base site of the catalyst captured α-H to promote the formation of enolate from n-butyraldehyde, and the Lewis acid sites promoted the dehydration of intermediate products. DFT simulation showed that n-butanol activated α-C in enolate in aldol condensation, and deactivated the oxygen atoms in enolate by hydrogen bonds to inhibit side reactions. Finally, the obtained condensation products were subjected to HDO reaction over the 5 wt% Pd/C and HZSM-5 catalysts, obtaining the highly branched alkanes with an ultra-low freezing point of -120.7 °C for C8 alkane and -78.7 °C for C12 alkane suitable for bio-jet fuels.
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EUROPEAN POLYMER JOURNAL
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2024
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IF 5.8
Yirong Fan,Tao Wang,Hui Sun
Metal ion coordination has critical influence on the self-assembly behavior of amphiphilic polymers and the morphology of the obtained assemblies. Herein, an amphiphilic homopolymer with 2,2′-bipyridine (BPy) as side chain is synthesized (noted as PBPyAA), which can self-assemble into bowl-shaped nanoparticles (BNPs) in tetrahydrofuran (THF)/water. Taking advantage of the coordination interaction between BPy and metal ions, Fe 2+ is chosen to regulate the self-assembly behavior and the morphology of the assemblies of PBPyAA in two pathways. (Ⅰ) The aqueous solution of Fe 2+ with various concentrations is added to the THF solution of PBPyAA during self-assembly. (Ⅱ) Fe 2+ is added into the THF solution of PBPyAA before self-assembly, followed by the addition of deionized water to promote the self-assembly. The results show that the pathway Ⅰ facilitates the coordination of BPy and Fe 2+ . With the increase of the concentration of Fe 2+ aqueous solution, the coordination efficiency of BPy increases from 0.419 % to 7.789 %, leading to the transformation of BNPs to vesicles. Though the coordination efficiency of BPy also increases with the concentration of Fe 2+ in pathway Ⅱ, which is still quite low of 0.274 % to 0.366 %, and the morphology of the BNPs barely changes. In addition, ethylene diamine tetraacetic acid (EDTA), a strong chelating agent, is also added to promote the competitive complexation with BPy, resulting in the dissociation of BPy and Fe 2+ and the reversible transformation from vesicles to BNPs. Overall, the effect of Fe 2+ coordination on the self-assembly behavior of PBPyAA in two pathways is investigated and the reversible transformation of BNPs to vesicles is also achieved.
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Cell Reports Physical Science
·
2025
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IF 7.3
Zhongzhe Wei,Xu Liu,Mingxuan Wang,Yao Lv,Songtao Huang,Jing Wang,Ming Jiang,Zhixiang Yang,Zihao Yao,Sheng Dai,Xiaonian Li,Jianguo Wang
The semi-hydrogenation of alkynes represents a paramount chemical transformation in the synthesis of fine chemicals and pharmaceuticals. However, the structural evolution of active sites during the reaction remains elusive. Here, we constructed a self-adaptive Pd/Nb 2 O 5 catalyst for efficient semi-hydrogenation of alkynes. Mechanistic studies disclose that Pd/Nb 2 O 5 intelligently modulates its structure in response to the specific alkyne type, efficiently preventing Pd poisoning by weakening the strong adsorption of alkynes. During the hydrogenation of aliphatic alkynes, the Pd/Nb 2 O 5 interface undergoes dynamic changes, generating oxygen vacancies (O v ) in situ through hydrogen spillover. In contrast, for the case of reactants of aromatic alkynes, the interface sites remain relatively stable. Coverage-dependent kinetics reveal that the dynamic O v formation of Pd/Nb 2 O 5 is determined by the distinct adsorption mechanism of aromatic and aliphatic alkynes. Due to the evolving interface, Pd/Nb 2 O 5 exhibits a high turnover frequency value of 55,338 h −1 , breaking the linear scaling relationships.
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