CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yaqian Dong,Zhi Fang,Deliu Ou,Qing Shi,Yu Ma,Weiyou Yang,Bin Tang,Qiao Liu
Constructing inexpensive, efficient, and stable pH-universal oxygen reduction electrocatalysts with controlled distribution of active species is of great importance for the exploration of green energy conversion devices. Herein, we demonstrated the rational preparation of S-modified Fe–N–C nanosheet catalysts with hierarchical porous architecture, large specific surface area (up to 1471 m 2 g −1 ) and controlled S doping (up to 12.3 at.%) by the co-pyrolysis of cysteine, FeCl 3 with Zn-mediated MgO template. Merited from rich and accessible active sites, the catalysts display outstanding oxygen reduction reaction (ORR) activity in terms of very small E j3 (potential@3 mA cm −2 , 0.87 V in 0.1 M KOH, 0.66 V in 0.1 M PBS (pH7.4) and 0.64 V in 0.5 M H 2 SO 4 ) and overwhelming diffusion-limited current density (9.8, 6.1, 10.3 mA cm −2 in alkaline, neutral, acidic media, respectively), along with extremely respectable stability (∼90% activity retention for 53200, 26728, 43200 s in alkaline, neutral, acidic media, respectively), which underscore comparable or even better overall performance than commercial Pt/C and advanced pH-universal ORR catalysts ever reported. The as-assembled primary alkaline zinc–air battery delivers considerately large peak power density of 205 mW cm −2 and energy density up to 990.6 Wh kg Zn −1 at 10 mA cm −2 (115 mW cm −2 and 676.7 Wh kg Zn −1 for Pt/C-based battery), implying its highly promising application in practical energy conversion devices.
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Small
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2024
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IF 13
Feng Sun,Zhihui Ma,Shenghai Xin,Yidi Fu,Ping Li,Jianbin Li,Qi Wan,Xuanhui Qu
Silicon (Si) anode is a promising anode material for all-solid-state lithium batteries with ultra-high theoretical specific capacity and low lithium dendrite risk. However, the inevitable vast volume expansion of Si anode during charge/discharge is recognized as a major limitation preventing its commercial application. Herein, an N, S self-doped amorphous carbon layer coated on porous micron-sized Si (p-mSi@C) is designed to construct an electron/ion conducting network while ensuring structural and interfacial stability. Uneven distribution of von mises stresses during p-mSi lithiation leads to irregular volume expansion and even fragmentation. Meanwhile, the growth of by-products at the interface between p-mSi and electrolyte contact leads to a rapid capacity decay. Compared to p-mSi anode, p-mSi@C reduces the risk of fragmentation thanks to the stress-absorbing effect of amorphous carbon, delivering excellent electrochemical performance (2679.65 mAh g −1 at 0.2 mA cm −2 with initial coulombic efficiency of 84%). More importantly, the chemical failure mechanisms of p-mSi and p-mSi@C composite anodes are revealed through structural characterization, chemical analysis, and simulation, which provides the necessary theoretical guidance for practicalization.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ming Xu,Yu Ma,Lei Wang,Shu Huang,Liming Chen,Rong Liu,Zikun Li,Guohui Yuan
Transition metal selenides (TMS) have been used to prepare hundreds of electrode materials for ion batteries due to their superior theoretical capacity, but have been repeatedly limited by the sluggish reaction kinetics and the enormous volume change during the repeated charge/discharge process. Here, we report a facile strategy to fabricate organic–inorganic composites by engineering a unique chemical bonding interface between TMS and conductive polymers. For the first time, poly(3,4-ethylenedioxythiophene) (PEDOT) is utilized to encapsulate iron diselenide (FeSe 2 ) nanoparticles by in situ polymerization, and the Fe-S bonds are meanwhile formed at the interface of FeSe 2 and PEDOT. The experimental analysis demonstrates the stability of Fe-S bonds during the sodiation/desodiation process and after long cycling, which can serve as a “bridge” for fast charge transfer and also serve as a “rivet” to stabilize the composite structure. When used for sodium ion storage, the composite offers an exceptionally long lifetime of up to 17,000 loops at 10 A/g without capacity degradation. In addition, it delivers a high specific capacity of 490.4 mAh/g and retains 60 % when the current density is amplified 150 times. The assembled full cell also exhibits excellent cycling stability. This work will provide a feasible way to improve the metal oxide/sulfide/selenides for long-life ion batteries.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jiangli Sun,Huizhong Wu,Chunhong Fu,Chaohui Zhang,Zhongzheng Hu,Minghua Zhou
A novel photoelectrocatalytic (PEC) system consisting of S-scheme MgO/g-C 3 N 4 photoanode and modified carbon felt (MCF) cathode was designed for efficient degradation of tetracycline , in which photoanode had both efficient photocatalytic performance and activation of H 2 O 2 produced by the MCF cathode. After 30 min of LED irradiation, the PEC system could completely remove tetracycline at cathodic bias of −0.5 V (vs. Ag/AgCl), and the degradation rate constants were 5.3 and 1.5 times that of electrocatalysis and photocatalysis . The charge transfer mechanism of S-scheme MgO/g-C 3 N 4 was verified by experimental studies and DFT calculations. Mg-N coordination was the key to activate H 2 O 2 to produce singlet oxygen ( 1 O 2 ) and hydroxyl radicals ( • OH). The PEC system had excellent degradation performance at pH ranges 4–10, which solved the bottleneck that Fenton system is effective at narrow pH range. This study provides new ideas for preparation of bifunctional photoanodes and new insights into the PEC process.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zhenhai Liu,Lei Duan
Iron sulfide nanoparticles (Nano-FeS) have shown great potential for in situ remediation of heavy metal and metalloid contamination from groundwater. However, limitations on mass transfer and efficacy of nano-FeS in the subsurface pose significant challenge. Herein, a reactive and efficient nano-FeS coating was developed in situ for the stabilization of metal(loid)s from groundwater. Alternate injection of FeSO 4 and Na 2 S can realize nano-FeS coating on sand grains with negligible changes in porosity, and the formation was dominated by growth and agglomeration process. Application scenarios for this nano-FeS coating include permeable reaction walls designed for preventive measures and in situ reaction zones that have experienced contamination. For the first scenario, the preformed nano-coating effectively sequesters As(III) through surface complexation and precipitation, and sequesters Cr(VI) through surface adsorption and reduction/precipitation. The retardation factor of As(III) and Cr(III) increased by 5.9 and 8.3 times, respectively, relative to the unamended sand. For the second scenario, we used alternate injection of FeSO 4 + heavy metal (Cd, Pb, and Cu) and Na 2 S to simulate the in situ immobilization of contaminants from real groundwater. The results showed that the alternating injection of Fe 2+ and HS − significantly enhanced the immobilization of heavy metals through both adsorption and direct interaction between heavy metals and HS − , with minimal detachment from the quartz sands. Overall, the findings highlight that in situ formation of nano-FeS coating as aquifer materials has significant potential as a cost-effective and straightforward groundwater remediation technology under environmentally relevant conditions.
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Nano Today
·
2024
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IF 13.2
Xue Wang,Lili Xia,Hui Cheng,Kexing Li,Wei Feng,Xinyue Dai,Yu Chen
Reactive oxygen species (ROS) can induce oxidative damage to biomolecules within tumor cells, making them suitable for tumor therapy. However, the effectiveness of these ROS in treating tumor cells is restricted due to their short half-life or short diffusion distance. Sulfate radicals (SO 4 • – ), with a longer half-life and higher oxidation potential , provide a compelling alternative. Herein, we propose an efficient strategy to activate peroxymonosulfate (PMS) and produce SO 4 • – and •OH by using ultrasound-mediated Cu 2+ /Cu + redox cycling, enabling oxygen-independent synergistic tumor therapy. Notably, this redox cycle ensures the continuity of effective Cu + catalytic sites and prevents adverse effects on healthy tissues. The density functional theory results demonstrate that the decisive copper valence-conversion step is derived from the ultrasound-induced excitations of electrons in spin-down bands of Cu 2 (OH)PO 4 . This ultrasound-controlled transition metal valence alteration enables in-situ activation of a nontoxic drug to produce toxic reactive X (X = O/S) species in an O 2 -independent manner, offering an efficient, adaptable and universal methodology for treating hypoxic tumors in living systems.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2024
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IF 1.5
Lei Miao,Zhang Jun,Liu Chang,Guo Junpeng,Li Ye
Herein, S-nZVI was synthesized to remove U(VI) from seawater. At a S/Fe ratio of 0.18 and pH of 5, adsorption of U(VI) reached equilibrium after 20 min with the removal rate of 97.93%. And the maximum adsorption capacity obtained by Langmuir isothermal model was 1177.09 mg/g. Moreover, S-nZVI exhibited selectivity in the presence of interfering ions, regeneration performance in 5 reuse cycles, and high removal efficiency in actual seawater. Mechanism investigations showed that UO 2 2+ uniformly adsorbed on S-nZVI surface was irreversibly reduced and generated UO 2 precipitates due to the electrons provided by S 2− , S 2 2− and Fe(II).
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Jing Zhang,Honghui Wang,Yingmin Liao,Yan Li
The co-contamination of heavy metal ions and organic pollutants has posed a threat to human health. Herein, this study investigated the intermolecular interactions of bisphenol S (BPS) and hexavalent chromium (Cr(VI)) under both individual and coexisting conditions, with alpha-glucosidase (AG), a key enzyme in carbohydrate metabolism, and the corresponding effects on the structure and function of AG. Multiple spectroscopic and molecular docking methods were employed to conduct the investigation in vitro and in silico . The results indicated that both BPS and Cr(VI) quenched the fluorescence of AG via a combined static and dynamic quenching processes. At 310 K, the binding constants of AG with BPS in the AG-BPS and (AG-Cr(VI))-BPS systems were 1.84 × 10 4 and 2.03 × 10 4 L mol −1 , and the binding constants of AG with Cr(VI) in the AG-Cr(VI) and (AG-BPS)-Cr(VI) systems were 6.14 × 10 3 and 4.35 × 10 3 L mol −1 . Cr(VI) could significantly affect the binding site of BPS in AG, while BPS had a minimal impact on the binding site of Cr(VI) in AG. BPS and Cr(VI) caused varied structural alterations of AG, and the impact of their coexistence on the structure of AG was related to the order in which they were added. Both BPS and Cr(VI) had a concentration-related effect on AG activity. This study provides valuable insights into the molecular mechanisms underlying the combined toxic effects of BPS and Cr(VI) on AG, highlighting the potential health risks associated with their environmental co-exposure.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Zhihan He,Linjia Li,Youyu Pang,Meng Cui,Yanhong Lin,Tengfeng Xie
The photocatalytic synthesis of hydrogen peroxide (H₂O₂) through the two-electron oxygen reduction reaction (ORR) presents a sustainable approach for the production of this industrially crucial compound. However, the photocatalytic efficiency is hindered by inefficient charge separation and sluggish interfacial reaction dynamics. In this study, we have fabricated Ag-modified sulfur vacancy-rich ultrathin ZnIn₂S₄ nanosheets (Ag-Sv-ZIS) as highly effective ORR catalysts, which display a H₂O₂ production rate of 8966 μmol g −1 h −1 under visible light irradiation (≥420 nm). In-situ transient surface photovoltage (TPV) spectra and femtosecond transient absorption (fs-TA) spectra indicate that the incorporation of Ag efficiently promotes the interfacial charge transfer between the photocatalyst and O₂. This research offers novel perspectives on the design of high-performance photocatalysts via the rational engineering of active sites and surface reaction dynamics for efficient photocatalytic H₂O₂ synthesis.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Cai-Yun Zhang,Chen-Yang Wang,En-Zhu Zhao,Guowei Yu,Hui-Ling Deng,Rui Huang,Zhao-Yun Wang,Pu Hu,Min Yan,Zhitian Liu
Lithium‑sulfur batteries demonstrate substantial promises for evolving into next-generation energy storage systems, but sluggish kinetics of LiPSs conversion and poor interfacial stability at the cathode-electrolyte interface remain critical challenges. Biowaste carbon as hosts is a cost-effective strategy to improve the electrical conductivity of Li-S batteries. However, limited polar sites in raw biowaste carbon restrict the capacity to anchor LiPSs. Herein, we propose a bio-derived hybrid host (PANI@GC) synthesized from waste grapefruit peels and polyaniline to address the rate-determining steps in sulfur electrochemistry. The grapefruit-derived carbon establishes an excellent conductive network that enables rapid electron transfer, while the PANI-integrated numerous polar sites (aromatic amine groups, conjugated π-π stacking) create a catalytically active interface to anchor and accelerate LiPSs conversion kinetics. Due to the conductive-catalytic network, the PANI@GC/S cathode delivers exceptional performance of 1190 mAh g −1 at 0.2C and maintains 779.8 mAh g −1 under stringent conditions (5 mg cm −2 sulfur loading, 8 μL mg −1 E/S ratio). Remarkably, the catalytic interface minimizes capacity fading, exhibiting only 28.9 mAh g −1 loss after 7-day rest, compared to Pure S (152.83 mAh g −1 ). This research pioneers a sustainable strategy to engineer conductive-catalytic networks at cathode-electrolyte interfaces, providing fundamental insights into biowaste utilization for high-energy-density battery systems.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Jin Liang,Tian Lei,YaXi Zhang,Ye Yuan,Guang Yang,Li Zhang
Metal–organic frameworks (MOFs) have gained widespread recognition as versatile catalyst precursors owing to their unique structural merits and straightforward synthetic accessibility. Herein, the UiO-66(Ce)/ZIF-67 composite MOF precursor was constructed through a hybridization strategy, and subsequently transformed into a nonprecious metal sulfide catalyst (denoted as CeS/CoSx) employing hydrothermal sulfidation. Benefiting from the CeS/CoSx architecturally engineered hollow polyhedral nanocage structure and strong electronic interaction between CeS and CoSx, the composite catalyst demonstrates significantly accelerated electron transfer kinetics and outstanding catalytic activity. In 1.0 M KOH, CeS/CoSx only necessitates an overpotential of 143 mV to achieve a current density of 10 mA cm–2 for the hydrogen evolution reaction (HER). Regarding the oxygen evolution reaction (OER), overpotentials of 250 and 291 mV were required to attain current densities of 10 and 50 mA cm–2, respectively. Remarkably, the assembled CeS/CoSx||CeS/CoSx two-electrode overall water splitting system requires only 1.60 V to achieve a current density of 10 mA cm–2. Moreover, during the 40 h continuous electrolysis test, the potential fluctuation remained within 1%. This study provides an effective strategy for designing high-performance, dual-MOF-derived sulfide composite bifunctional electrocatalysts.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Cuihuan Lv,Jinpeng Cai,Guohui Wang,Jiuxiu Chen,Hao Lai,Peilun Shen,Dianwen Liu
Organic depressants often exhibit low selectivity at high dosages, and introduce risks of concentrate dewatering. The combined depressants composed of inorganic and organic substances can significantly reduce reliance on organic depressant dosage, providing a promising solution to this challenge. In order to achieve highly efficient separation of sphalerite and pyrite in the CuSO 4 -butyl xanthate (PBX) flotation system, the combined depressant Fe 2+ / baicalin (BCL) was innovatively employed to inhibit copper-activated pyrite. The flotation tests indicate that compared with the single depressant BCL, the combined depressant Fe 2+ /BCL demonstrates superior selective inhibitory effects on copper-activated pyrite. For artificially mixed ores, a zinc concentrate is obtained with a zinc grade of 62.33 % and a zinc recovery of 93.86 % when the combined depressant of 10 mg/L Fe 2+ and 5 mg/L BCL are used, and the separation efficiency is significantly improved from 40.66 to 79.69 %. Adsorption characteristic studies indicated that BCL exhibits stronger affinity for copper-activated pyrite than for sphalerite. The introduced Fe 2+ provide additional active sites, thereby enhancing the depression effect on copper-activated pyrite. Following Fe 2+ /BCL modification, the adsorption of PBX on copper-activated pyrite was hindered, while having no substantial impact of that on sphalerite, which is also confirmed by molecular dynamics simulations. Therefore, the combined depressant Fe 2+ /BCL markedly widened the hydrophobicity difference between sphalerite and pyrite, creating the potential for their effective separation.
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