JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yaning Du,Yangai Liu,Bing Zhu,Qingyu Zhang,Zhaofeng Tian
The practical application and development of lithium-sulfur batteries (LSBs) remains a serious issue as a consequence of the shuttle effect of lithium polysulfides (LiPSs). Halloysite (HNT), a clay mineral with a unique hollow tubular structure, is a potential carrier for sulfur. In this work, we employed a strategic approach to modify both inner and outer surfaces of HNT. We synthesized N-doped carbon-coated thin-wall hollow nanotube HNT composites (A 5 HNT@NC), which were subsequently utilized as sulfur carriers in the cathode of LSBs. This method alleviates the shuttle effect of LiPSs and controls the volume expansion of sulfur during charge-discharge. Acid heat treatment reduced Al-O octahedron in HNT, expanding the inner diameter to enhance the loading of sulfur. A 5 HNT@NC, prepared through phase inversion and high-temperature pyrolysis, effectively enhanced the electrical conductivity of thin-walled HNT, facilitating Li + and electron transfer. Meanwhile, the structure of A 5 HNT@NC effectively adapted volume expansion of sulfur, realized high sulfur loading, and provided abundant active sites for anchoring of LiPSs. Moreover, the incorporation of N elements on carbon layer enhanced the ability to catalyze and adsorb LiPSs. Consequently, A 5 HNT@NC/S cathode exhibited high cycle stability and specific capacity. At 0.2 C, it retained high capacity of 619.7 mAh g −1 after 100 cycles, achieving 84.67 % capacity retention. At a higher current density of 0.5 C, A 5 HNT@NC/S cathode also retained specific capacity of 515.0 mAh g −1 after 300 cycles. This work can expand the application of HNT for energy storage, provide inspiring insights into the design of novel sulfur carrier materials for LSBs.
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CHINESE CHEMICAL LETTERS
·
2025
·
IF 8.9
Ziyun Li,Di Shen,Qi Liu,Hongtu Shi,Tianyu Han,Jie Jiang,Xu Zhang,Yu Fu,Lei Wang
The electrocatalytic two-electron oxygen reduction reaction (2e – ORR) offers an environmentally friendly method for hydrogen peroxide (H 2 O 2 ) production, yet the development of efficient and cost-effective electrocatalysts remains a significant challenge. Herein, we have synthesized Ni 3 N 2 clusters anchored on N-doped carbon nanostructures (Ni 3 N 2 /NC) through a straightforward biomass-derived modification-pyrolysis method for efficient H 2 O 2 production. Theoretical calculations reveal that the d-band center of Ni sites in Ni 3 N 2 /NC shows a downshift and successive state, which is beneficial to the formation of key *OOH intermediates and occurrence of subsequent reactions. Remarkably, Ni 3 N 2 /NC achieves a 2e – ORR selectivity of 91.65% and an onset potential of 0.69 V. When tested in a practical flow cell, Ni 3 N 2 /NC exhibits a Faradaic efficiency (FE) of 91.42 % and attains a maximum H 2 O 2 yield of 3.26 mol g cat −1 h −1 at 100 mA/cm 2 . Additionally, the FE remains above 85% during a 12 h constant current stability test at 40 mA/cm 2 , highlighting its potential for sustainable H 2 O 2 production.
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WATER RESEARCH
·
2024
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IF 11.4
Peizeng Yang,Hailing Chu,Jiating Liu,Teng Zhang,Junhe Lu
Sulfate radical (SO 4 •− ) advanced oxidation processes (SR-AOPs) are efficient for degrading a broad spectrum of contaminants. This study demonstrates that the existence of environmentally relevant concentrations of nitrite (NO 2 − ) can lead to the formation of N -nitrosodimethylamine (NDMA), a probable human carcinogen, when heat activated peroxydisulfate (heat/PDS) is applied to address contaminants with dimethylamine moieties, such as tetracyclines. NO 2 − effectively competes with tetracyclines for SO 4 •− at a high second-order reaction rate constant of 8.8 × 10 8 M −1 s −1 , thus suppressing the degradation. Simultaneously, SO 4 •− reacts with NO 2 − to form the nitrogen dioxide radical (NO 2 • ) which rapidly dimerizes to a potent nitrosating agent named dinitrogen tetroxide (N 2 O 4 ). N 2 O 4 , in turn, attacks the dimethylamine moiety in tetracyclines via nucleophilic substitution, contributing to the degradation of parent compounds and generating an active intermediate that quickly decomposes to NDMA, along with the release of R + and NO 3 − . The released R + can be further oxidized by SO 4 •− to form phenolic intermediates which combine with NO 2 • to generate nitrated products. When 5 μM oxytetracycline (OTC) was treated with 0.5 mM PDS in the presence of 20 μM NO 2 − at 60 °C, the highest formation of NDMA was 0.045 μM in 1 h. NDMA formation was also observed for other compounds with dimethylamine moieties, such as methylene blue, phenylurea herbicides, etc., with the molar yield ranging from 0.07 to 3.53 %, negatively related to the R-N bond dissociation energy of the precursors. These findings suggest that NDMA can be commonly generated when SO 4 •− is applied to the degradation of dimethylamine pollutants in wastewater treatment or groundwater remediation where NO 2 − ubiquitously exists, which may pose a serious threat to the aquatic environment.
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OPTICAL MATERIALS
·
2024
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IF 3.8
Shutong Chen,Xiaosan Song,Xichen Song,Yue Zhang
This study involved the synthesis of modified ZnO materials for photoelectrocatalysis (PEC) by a simple and environmentally friendly electrochemical procedure. The objective was to assess their capacity to photochemically breakdown ofloxacin (OFX) in an aqueous solution. To enhance the PEC performance of pure ZnO, a zinc oxide–reduced graphene oxide (ZnO–rGO) composite was synthesized through an electrochemical co-deposition process without the use of a reducing agent. Subsequently, ZnO–rGO was doped with N (ZnO–rGO:N) to further augment the PEC performance of the photoanode. The surface morphology, microstructure, and optical characteristics of the materials were systematically investigated through X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and UV–visible spectroscopy. The parameters for synthesizing ZnO–rGO were optimized based on the experimental results” if it can more simply convey your intended meaning. Electrochemical tests demonstrated that N-doping significantly enhanced the photocurrent density of the ZnO–rGO films, which reached 15.14 μA cm −2 , representing 1.6- and 1.3-fold enhancements with respect to those of pure ZnO (9.25 μA cm −2 ) and ZnO–rGO (12.0 μA cm −2 ), respectively. Additionally, the band gap in ZnO was narrowed from 3.4 to 3.18 eV owing to rGO co-deposition and N-doping. After 180 min of Xe lamp irradiation, with a bias potential of 0.7 V (referenced to Ag/AgCl), ZnO–rGO:N demonstrated an OFX degradation rate of 55.7 %. Thus, the N-doped material exhibited higher PEC performance than either ZnO (31.8 %) or ZnO–rGO (36.3 %), implying its enhanced PEC capabilities. Therefore, the modified ZnO-based photoanode prepared using the straightforward electrochemical deposition method satisfied the objective of this study, which was to enhance its PEC activity while providing a viable foundation for nitrogen doping through electrochemical methods.
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FUEL
·
2024
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IF 6.7
Man Lang,Dengwei Wang,Shenbo Yang,Hao Li
The development of excellent performance catalysts for the hydrodeoxygenation of renewable biomass into value-added chemicals is essential but remains extremely challenging. Herein, a series of novel metal-free carbo-catalyst catalysts through one-step-pyrolysis strategy were fabricated for the hydrodeoxygenation (HDO) of lignin-derived vanillin (VAN) to produce 2-methoxy-4-methylphenol (MMP). It has been demonstrated that 81.32 % VAN conversion could be acquired with a high selectivity of 77.30 % of MMP under the condition of 240 °C, 1 MPa H 2 and 4 h with the assistance of the optimized NSCC-800-7 catalyst. After characterization of the catalyst and density functional theory (DFT) calculations, the outstanding catalytic activity is attributed to the synergistic effect between nitrogen and sulfur dopants, which effectively regulates the number of active sites. N-S vacancy (NSVs) in the N-doped carbon catalysts is found to play an active site for the VAN HDO reaction, which is greatly beneficial to activating hydrogen molecules. Meanwhile, sulfur doping can promote the formation of defect sites and high specific surface area, while enabling to stabilization of NSVs. Additionally, isopropanol was both the reaction medium and the secondary hydrogen donor, which contributed to reducing the external hydrogen supplication. This finding can open broad opportunities for the rational design of novel metal-free catalysts for challenging chemical reactions.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Shen Jiafu,Huang Xi,Dai Yu,Zhang Xiaojin,Xia Fan
Low-grade heat is abundant and ubiquitous, but it is generally discarded due to the lack of cost-effective recovery technologies. Ion thermoelectric cells are an affordable and straightforward approach of converting low-grade heat into usable electricity for sustainable power. Despite their potential, ion thermoelectric cells face challenges such as limited Seebeck coefficient and required series integration. Here, we demonstrate that the N-type and P-type conversion of ion thermoelectric cells can be achieved through the phase transition of temperature-sensitive hydrogel containing the triiodide/iodide redox couple. Through the strong interaction between the hydrophobic region of the hydrogel and triiodide, the hydrophobic side selectively captures triiodide and the hydrophilic side repels triiodide, raising the concentration difference of triiodide and thereby increasing the Seebeck coefficient. Specifically, the Seebeck coefficient of the N-type ion thermoelectric cells is 7.7 mV K −1 , and the Seebeck coefficient of P-type ion thermoelectric cells is −6.3 mV K −1 (Δ T = 15 K). By connecting 10 pairs of the N-type and P-type ion thermoelectric cells, we achieve a voltage of 1.8 V and an output power of 85 μW, surpassing the reported triiodide/iodide-based ion thermoelectric cells. Our work proposes a phase transition strategy for the N-P conversion of ion thermoelectric cells, and highlights the prospect of series integrated hydrogel ion thermoelectric cells for low-grade heat harvesting.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Qianqian Song,Yang Chen,Yongjian Xu,Yatao Yan,Qianhui Wu,Fang Guo,Ming Chen,Guowang Diao
Hydrogen energy represents a form of green energy, and the electrolysis of water for hydrogen production is recognized as an efficient method. Current research is primarily focused on the development of catalysts that are both efficient and stable, particularly those capable of functioning consistently across the entire pH spectrum. In this work, Co 9 S 8 /NC co doped with N and P was successfully synthesized through a series of sulfurization, calcination, and phosphating operations using dual ligand Co-ZIF as the precursor. By coating a carbon layer and co doping with nitrogen and phosphorus, the catalytic performance and stability of hydrogen evolution reaction (HER) were significantly improved over the entire pH range. At a fixed current density of 10 mA cm −2 , the overpotential of HER was measured at voltages of 136, 96, and 194 mV in three different pH solutions. Furthermore, the electrocatalyst exhibits remarkable electrochemical stability over extended periods. After 20 h or 2000 cycles of testing, the catalytic activity did not show a significant decrease across the entire pH range, but rather exhibited a relatively sustained constant.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Ziyan Pu,Zengquan Zhu,Xiao-Jun Lv,Yueming Li
Conventional lithium-ion batteries (LIBs) are nearing their theoretical capacity limit, and there is an urgent need to develop energy storage devices with higher energy densities and cycling stabilities. In this work, a hybrid electrode design, which combines the traditional “rocking chair” mechanism and “anion intercalation” mechanism to improve energy density is reported. The hybrid electrode is composed of LiMn 2 O 4 and N,P-doped graphite (NPG) to use both anion and cation storage mechanisms. This design enhances the electrochemical potential windows and the energy density of the fabricated cell. Electrochemical results show that the fabricated cell not only shows a 44.1 % higher capacity than conventional LIBs. It displays a stable cycle life across a wide climate temperature range from − 20 to 25 °C, with a capacity retention rate of 86 % after 600 cycles at 100 mA g −1 . This study demonstrates the critical role of doping graphite with N and P to improve the electrochemical performance of graphite in deep charge/discharge, providing a valuable strategy for developing cathode materials in dual-ion batteries.
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NEW CARBON MATERIALS
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2024
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IF 6.5
Tan Yi,Jun-long Huang,Zong-heng Cen,Yi-wei Ji,Shao-hong Liu
Carbon-based catalysts are promising materials for the electrochemical extraction of uranium from seawater. However, their practical application is often limited by high cost and low catalytic activity. Using low-cost polystyrene sulfonic acid resin and melamine as raw materials, a class of nitrogen and sulfur co-doped carbon nanosheets (CNSs) with high catalytic activity has been developed by a low-temperature hydrothermal treatment and high-temperature carbonization. Because of their high conductivity and high catalytic activity, CNS-based electrodes can catalyze uranyl ions in seawater into easily recoverable Na 2 O(UO 3 ·H 2 O) x precipitates at −2 V, and achieve an extraction capacity of up to 3 923.7 mg g −1 with a uranium removal of 98.1% in uranium-spiked seawater (1×10 3 mg L −1 ). In situ Raman spectroscopy showed that a large number of uranium compounds appeared on the surface of the composite electrode within 40 min of extraction. The electrode also recovered 72.7% of the uranium in natural seawater, demonstrating excellent prospects for this application. This work provides a new approach into the design of low-cost, metal-free electrocatalysts for the efficient uranium extraction from natural seawater.
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CANCER SCIENCE
·
2024
·
IF 4.5
Luhaoran Sun,Zeyu Li,Peng Shu,Min Lu
High expression of truncated O-glycans Tn antigen predicts adverse clinical outcome in patients with clear cell renal cell carcinoma (ccRCC). To understand the biosynthetic underpinnings of Tn antigen changes in ccRCC, we focused on N-acetylgalactosaminyltransferases (GALNTs, also known as GalNAcTs) known to be involved in Tn antigen synthesis. Data from GSE15641 profile and local cohort showed that GALNT6 was significantly upregulated in ccRCC tissues. The current study aimed to determine the role of GALNT6 in ccRCC, and whether GALNT6-mediated O-glycosylation aggravates malignant behaviors. Gain- and loss-of-function experiments showed that overexpression of GALNT6 accelerated ccRCC cell proliferation, migration, and invasion, as well as promoted ccRCC-derived xenograft tumor growth and lung metastasis. In line with this, silencing of GALNT6 yielded the opposite results. Mechanically, high expression of GALNT6 led to the accumulation of Tn antigen in ccRCC cells. By undertaking immunoprecipitation coupled with liquid chromatography/mass spectrometry, vicia villosa agglutinin blot, and site-directed mutagenesis assays, we found that O-glycosylation of prohibitin 2 (PHB2) at Ser161 was required for the GALNT6-induced ccRCC cell proliferation, migration, and invasion. Additionally, we identified lens epithelium-derived growth factor (LEDGF) as a key regulator of GALNT6 transcriptional induction in ccRCC growth and an upstream contributor to ccRCC aggressive behavior. Collectively, our findings indicate that GALNT6-mediated abnormal O-glycosylation promotes ccRCC progression, which provides a potential therapeutic target in ccRCC development.
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Cell Death Discovery
·
2024
·Vol. 10
·期 1
·1-16
·
IF 6.1
Liu Zhaohong,Xiang Peng,Zeng Shengmei,Weng Ping,Wen Yilin,Zhang Wanping,Hu Hui,Zhao Dezhang,Ma Limei,Yu Chao
Vascular endothelial injury initiates atherosclerosis (AS) progression. N -Acetylneuraminic acid (Neu5Ac) metabolic disorder was found to intensify endothelial mitochondrial damage. And GLS2-associated glutaminolysis disorder contributed to mitochondrial dysfunction. However, mechanisms underlying Neu5Ac-associated mitochondrial dysfunction as well as its association with GLS2 remains unclear. In this study, we constructed GLS2 −/− ApoE −/− mice by using HBLV-GLS2 shRNA injection. And methods like immunofluorescence, western blotting, transmission electron microscopy were applied to detect profiles of endothelial injury and AS progression both in vivo and in vitro. We demonstrated that Neu5Ac accumulation increased GLS2 expression and promoted glutaminolysis disorder, which further induced endothelial mitochondrial dysfunction via a pyroptosis-dependent pathway in vivo and in vitro. Mechanically, Neu5Ac interacted with SIRT3 and led to FOXO3a deacetylation and phosphorylation, further facilitated c-Myc antagonism and ultimately increased GLS2 levels. Inhibition of GLS2 could improve mitochondrial function and mitigate pyroptosis process. In addition, blocking Neu5Ac production using neuraminidases (NEUs) inhibitor could rescue endothelial damage and alleviate AS development in ApoE −/− mice. These findings proposed that Neu5Ac induced GLS2-mediated glutaminolysis disorder and then promoted mitochondrial dysfunction in a pyroptosis-dependent pathway. Targeting GLS2 or inhibiting Neu5Ac production could prevent AS progression.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jinsong Shi,Jianguo Xu,Hongmin Cui,Nanfu Yan,Runhan Yan,Yaqing Weng
Porous carbon is a very promising type of CO 2 adsorbent due to its excellent stability, low cost, and tunable physicochemical properties. In the current work, N-doped hierarchically porous carbon was synthesized with the assistance of NaCl template and KHCO 3 activation. A series of carbons with three dimensional and interconnected micro- meso -macroporous structure were successfully prepared. Effects of synthesis conditions on textural properties and N-doping were analyzed and discussed with details. The carbons also exhibited high surface area (725–2423 m 2 /g) and N content (1.49–7.93 wt%). CO 2 adsorption properties were studied with a combined experimental and theoretical approach. At 25 °C and 1 bar, the carbons exhibited CO 2 uptake up to 4.22 mmol/g and CO 2 /N 2 selectivity up to 25.6. Grand canonical Monte Carlo (GCMC) simulation was employed to further elucidate the different roles played by N-doping and textural properties during CO 2 adsorption. Effects of various N-functionalities located in pores with different sizes on CO 2 adsorption were thus revealed. The present study presents a novel strategy for controlled synthesis of porous carbons, and provides helpful insights into their CO 2 adsorption behaviors.
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