GREEN CHEMISTRY
·
2024
·
IF 9.3
Genyan Hao,Tao Zhao,Qiang Fang,Yunzhen Jia,Dandan Li,Dazhong Zhong,Jinping Li,Qiang Zhao
Exploring Earth-abundant and efficient electrocatalysts to replace Ir and Ru for the acidic oxygen evolution reaction (OER) is essential to reduce the cost of clean hydrogen production. Here, we show that trace amounts of electronegative non-metallic element fluorine (F)-doped Co3O4 nanoneedles improve the activity and stability of Co3O4. The F-doped Co3O4 nanoneedles supported on carbon paper (F-Co3O4/CP) exhibit an overpotential of 350 mV at 10 mA cm−2 for the acidic OER. In addition, their performance remains consistent after continuous operation for 80 h. Detailed investigations reveal that introducing an anion promotes the enrichment of OH on the surface of Co3O4 and prevents acid corrosion, thereby enhancing the intrinsic OER activity and stability. Theoretical calculations further indicate that F doping can effectively improve electron transfer and optimize the energy barrier for the formation of *OOH intermediates, which significantly improves OER performance. This study provides guidance for designing efficient and stable non-noble metal acidic water oxidation catalysts.
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高影响因子
ADVANCED ENGINEERING MATERIALS
·
2024
·
IF 3.4
Fei Chen,Chengbao Liu,Leizhi Zheng,Feng Chen,Junchao Qian,Yongbin Qiu,Xianron Meng,Zhigang Chen
Nickel hydroxide (Ni(OH) 2 ) is recognized as a promising material for electrodes in supercapacitors owing to its exceptional theoretical specific capacitance. However, Ni(OH) 2 has several drawbacks, including a short cycle life, susceptibility to volume expansion, and poor electrical conductivity. In this work, Ni(OH) 2 nanosheets anchored on layered g-C 3 N 4 /C (Ni(OH) 2 –g–C 3 N 4 /C) are designed by biological template induction and a hydrothermal method. Ni(OH) 2 –g–C 3 N 4 /C has unique petal-like structures, which can provide a vertical charge transport channel to increase reaction potential of the material during the charge–discharge process. The introduction of biomass carbon can solve the problem of the bulk phase accumulation of g-C 3 N 4 and can also improve the overall conductivity of the composite. Compared to Ni(OH) 2 (522 F g −1 ), g-C 3 N 4 /C (76.2 F g −1 ), and g-C 3 N 4 (16 F g −1 ), the Ni(OH) 2 –g–C 3 N 4 /C-0.75 (NGC-0.75) composite exhibits the highest specific capacitance of 1034 F g −1 at 1 A g −1 . Furthermore, after 5000 cycles at 5 A g −1 , the capacitance of the material is maintained at 85.97%. Meanwhile, the asymmetric supercapacitor based on the NGC-0.75 shows a high energy density of 18.29 Wh kg −1 at the power density of 400.02 W kg −1 with excellent cyclic stability of 127.45% over 10 000 cycles.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jian Zhang,Jia-Fang Xie,Jie-Jie Chen,Wen-Wei Li,Jia-Cheng E. Yang,Yu-Ming Zheng,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS) activation is of great potential for sustainably degrading antibiotics included emerging contaminants from water. However, developing synthetic metal catalysts with incompatible mass transfer and optimized metal sites to effectively enable low-levels PMS activation and antibiotics removal is challenging. Herein, a protein-like Co catalyst of spatially hierarchical hydrophilicity is synthesized by constructing flower-like Mg/Al layered double hydroxide (LDH) on super-active carbon (AC) to disperse thin-layer Co(OH) 2 along the edge of LDH. The resulting AC-LDH@Co(OH) 2 catalyst demonstrates an impressive antibiotic removal of ≈80% within 15 s and turnover frequency of 45.72 min −1 based on catalyst mass by activating 0.075 mM PMS, surpassing single-atom catalysts included reports. In a fixed-bed reactor with secondary wastewater effluent, AC-LDH@Co(OH) 2 realizes complete removal of norfloxacin for 66 h with neutral effluent pH and negligible metal leaching. Experiments combined with theoretical computations reveal that the protein-like complex not only accelerates transfer of low-levels hydrophilic PMS and hydrophobic antibiotics, but also stably confines Co sites with regulated electronic structure for multiply reactive oxygen species generation.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Jiankang Wang,Yajing Wang,Yuan Peng,Zhongping Yao,Peng Zhang,Taiping Xie
The limited mass transfer and sluggish reaction kinetics of traditional powder catalysts, as well as the trade-off between permeate flux and the removal efficiency of confined membranes, have significantly hindered practical application in wastewater treatment. In this work, a Co 2 CO 3 (OH) 2 /polyvinylidene fluoride (Co 2 CO 3 (OH) 2 /PVDF) confined catalytic membrane was constructed via a one-step hydrothermal method and used as a peroxymonosulfate (PMS) activator for tetracycline (TC) degradation. Surprisingly, Co 2 CO 3 (OH) 2 /PVDF achieved 99.67 % TC removal under continuous flow-through mode with an extremely short hydraulic retention time of 5.4 ms and a high permeate flux of 7085.5 L m −2 h −1 bar −1 . Furthermore, the reaction kinetic constant was five orders of magnitude higher than that under batch mode (1.07 ms −1 vs 0.37 min −1 ), demonstrating the superiority of membrane-confined catalysis in enhancing TC removal. Reactive oxygen species (ROS) scavenging experiments, electron paramagnetic resonance (EPR) spectra and electrochemical measurement revealed that the oxidative degradation of TC was dependent on cooperative attack of radicals (SO 4 • − , •OH and O 2 • − ) and non-radicals ( 1 O 2 ). Subsequently, three possible degradation pathways were proposed. This study highlighted the significance of confined effect and Co(Ⅱ) catalysis in synergistically promoting PMS activation for ultrafast TC removal, demonstrating the potential application of membrane-confined catalysis in industrial wastewater treatment.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2025
·
IF 4.7
Hezheng Sun,Guoqing Liu,Yi Zhao,Jingcun Shao,Changhui Xin,Yanting Tang,Xin Yu
Bisphenol A is an environmental hormone that shows a significant impact on human health. The removal of bisphenol A substances from the surrounding environment is of great significance for the humanity sustainable development. Current work focuses on synthesizing self-doped Nb 3 O 7 (OH) nanostructure and eosin Y/Nb 3 O 7 (OH) composites with high surface areas through a solvothermal process for bisphenol A degradation under visible-light illumination. The prepared Nb 3 O 7 (OH) sample demonstrated a noticeable photocatalytic performance toward bisphenol A degradation. Notably, the obtained eosin Y/Nb 3 O 7 (OH)-1.0 % composite not only exhibited efficient visible-light harvesting and high surface area but also showed significantly improved charge separation and bisphenol A degradation compared to pristine Nb 3 O 7 (OH) sample. The rate constant of the eosin Y/Nb 3 O 7 (OH)-1.0 % sample for bisphenol A degradation was approximately 0.04252 min −1 , which was 7.85 times that of pristine Nb 3 O 7 (OH) sample. Furthermore, the eosin Y/Nb 3 O 7 (OH)-1.0 % composite achieved approximately 59.76 % mineralization of bisphenol A within 20 min and 75.28 % mineralization within 40 min under visible-light illumination. Additionally, the effects of experimental parameters on bisphenol A degradation and the dye-sensitization mechanism were proposed. The current work suggests the obvious advantages of defective Nb 3 O 7 (OH) nanostructure in fabricating high-performance composite photocatalysts for eliminating emerging pollutants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Chunyu Zhang,Guang Yang,Xueqing Gao,Zhiyun Li,Yifan Li,Siyuan Wang,Junyong Wang,Xunhua Zhao,Kai Zhang,Yu Kang,Yi Cui
Surface OH species on electrocatalysts play a pivotal role in affecting the hydrogen evolution reaction (HER). Herein, we highlight the critical role of surface OH basicity in regulating interfacial water structure and OH desorption behavior. By annealing Ru/Ni(OH) 2 at various temperatures, we successfully tailored the electronic state of surface OH species, with the catalyst annealed at 300 °C (Ru-Ni-300) exhibiting superior HER performance, achieving a current density of 100 mA/cm 2 at an exceptionally low overpotential of 71 mV. X-ray photoelectron spectroscopy demonstrates that the electron-rich surface OH species on Ru-Ni-300 exhibit strong Lewis basicity. The enhanced OH basicity facilitates the formation of hydrogen-bond networks with interfacial water through electron donation, which in turn promotes OH desorption kinetics. Quasi-in-situ XPS and density functional theory calculations further elucidated that the increased electron density on surface OH species reduces OH adsorption energy, thus accelerating HER performance. These findings unveil a direct correlation between surface OH basicity and HER efficiency, offering new insights into tailoring surface environments for advanced water-splitting electrocatalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Leilei Yin,Yuyan Liu,Shuai Zhang,Jin-Cheng Liu,Yong Jiang,Yaping Du
Excessive adsorption of oxygen-containing intermediates during oxygen reduction reactions (ORR) on palladium (Pd)-based materials is a critical factor limiting their catalytic activity. Alloying presents a powerful strategy to overcome this inherent challenge. In this study, the alloying of the low electronegativity lanthanide gadolinium (Gd) with Pd is explored. Pioneering theoretical calculations indicate that Gd, acting as an electron donor, induces charge redistribution between the metals. This process weakens the over-adsorption of OH* intermediates on the Pd surface and reduces the reaction overpotential. Subsequent experiments yield Pd 3 Gd solid-solution nano-alloys supported on conductive carbon black (Pd 3 Gd/C-600), resulting in a 30 mV enhancement in half-wave potential and a 4.5 fold increase in mass activity in an alkaline medium compared to Pd/C-600. Due to its superior performance in ORR, Zn-air batteries utilizing Pd 3 Gd/C-600 cathodes demonstrate remarkable peak power density and stability over 330 h. This study offers valuable insights into the rational design of rare earth alloys and their catalytic chemistry in ORR.
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POLYMER BULLETIN
·
2025
·
IF 4
Zhang Chengpeng,Bei Pengzhi,Liu Hongjing,Zhao Xu,Shi Meiling,Jing Xiaochun,Li Zhao,Yao Hui
A novel porous liquid, M2070-UiO-66-OH@[BMim][PF 6 ], has been synthesized using zirconium-based metal–organic framework (UiO-66-OH), 1-butyl-3-methylimidazolium hexafluorophosphate ([BMim][PF 6 ]) and polyetheramine M2070. To enhance the CO 2 separation performance, M2070-UiO-66-OH@[BMim][PF 6 ] was incorporated as a filler into a mixed matrix membrane (MMM) using polyether block amide (Pebax-1657) as the membrane matrix. The properties of the synthesized M2070-UiO-66-OH@[BMim][PF 6 ] and the resulting MMMs have been characterized through FTIR, TGA, DSC, and SEM analyses. The results of porous liquid stability revealed that grafting polyetheramine M2070 onto the surface of UiO-66-OH@[BMim][PF 6 ] significantly increased the steric hindrance, thereby preventing agglomeration within the membrane. Additionally, the functional groups (amino and ether) present in M2070-UiO-66-OH@[BMim][PF 6 ] contributed to an increased number of active sites for CO 2 adsorption, facilitating enhanced CO 2 transport through the membrane. Compared to the Pebax membrane, the MMM containing 3% M2070-UiO-66-OH@[BMim][PF 6 ] exhibited significantly improved CO 2 permeability of 104.07 Barrer (an increase of 73.22%) and CO 2 /N 2 selectivity of 92.37 (an increase of 148.95%) at 30 °C and 0.3 MPa, surpassing the 2008 Robeson upper bound. These findings suggest that M2070-UiO-66-OH@[BMim][PF 6 ] is a highly promising additive for the fabrication of mixed matrix membranes with superior CO 2 separation performance. Graphical abstract A porous liquid, (M2070-UiO-66-OH@[BMim][PF 6 ]) has been prepared using UiO-66-OH@[BMim][PF 6 ] as the core and polyetheramine M2070 as the canopy. Afterwards, M2070-UiO-66-OH@[BMim][PF 6 ] has been added to the Pebax matrix to prepare M2070-UiO-66-OH@[BMim][PF 6 ]/Pebax mixed matrix membranes, which have been subjected to gas separation studies.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Mengyin Liao,Chao Wang,Xuanhua Zhang,Chao Luan,Wenyuan Xu,Zhongyi He
Novel Pt/Co(OH)2-NiO/C catalysts based on carbon black were successfully synthesized using the hydrazine hydrate reduction method and galvanic replacement strategies. They were subsequently tested for their activity in the electrocatalytic oxidation of methanol. It was observed that the peak current density of Pt/Co(OH)2-NiO/C (8.29 A mg-1Pt) was 22.4 times higher than that of commercial Pt/C-JM (0.37 A mg-1Pt). The electrocatalytic activities and durabilities of the synchronously synthesized Pt/Co(OH)2-NiO/C catalysts were significantly better than those of PtCo/C, PtNi/C, and PtCoNi/C-X (X = 200, 400, 600) catalysts synthesized by calcination in Ar at different temperatures. The reason is that the highly dispersed Pt helps to expose more active sites on the catalyst surface, and the addition of Co(OH)2 and NiO alters the electron density of Pt, which reduces the adsorption of intermediate CO, attenuates the toxic effect, and enables more efficient oxidation of methanol.
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ChemSusChem
·
2021
·Vol. 14
·期 16
·3382-3390
·
IF 8.928
Ting Feng,Jing Ding,Haiyan Li,Wei Wang,Bohua Dong,Lixin Cao
Graphical In hot water : CeO 2 /A−Fe(OH) 3 composites synthesized by a secondary water bath at 100 °C exhibit superior photocatalytic activity. A−Fe(OH) 3 increases specific surface area, passivates the surface of CeO 2 , and reduces the activation energy of water oxidation. This work provides a new insight into exploring amorphous cocatalysts to enhance photocatalytic O 2 evolution activity and augment the possibility of overall water splitting based on CeO 2 . Noble-metal-free composites with good photocatalytic property are of great interest. Here, CeO 2 nanorods composites loaded with amorphous Fe(OH) 3 cocatalyst were designed and prepared via a secondary water bath at 100 °C. The as-synthesized CeO 2 /amorphous Fe(OH) 3 composites exhibited superior light photocatalytic activities compared to pure CeO 2 , especially the sample with a loading time of 60 min. The photocatalytic oxygen generation rate could reach to 357.2 μmol h −1 g −1 , and the average apparent quantum yield (AQY) was 24.67 %, which was a 5.5-fold increase compared to the CeO 2 sample. The improvement of photocatalytic performance could be ascribed to three main reasons: First, loading the amorphous Fe(OH) 3 enlarged the specific surface area and passivated the surface of the pristine CeO 2 . Second, the amorphous Fe(OH) 3 ,which acted as a cocatalyst, provided many active sites, and reduced the reaction activation energy. Thirdly, the maximum interface with intimate contact between CeO 2 and amorphous Fe(OH) 3 cocatalyst accelerated the photogenerated charge separation efficiency and thus improved the photocatalytic performance of CeO 2 in photocatalytic water oxidation.
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PubMed
高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
·
2020
·Vol. 22
·期 2
·1-12
·
IF 2.132
Sun Xueying,Li Siqi,Liu Rongmei,Sun Xiulun,Liu Xinjie,Li Anran,Li Wen
In this work, we designed a simple hydrothermal synthetic method for a ZnCo-PBA@α-Co(OH) 2 nanosphere@nanosheet material with good electrochemical properties. The obtained material had a specific capacitance of 423.92 F g −1 at 1 A g −1 and a cycling retention ratio of 78.48% after 1000 cycles at 5 A g −1 . A hybrid supercapacitor device (ZnCo-PBA@α-Co(OH) 2 //AC) assembled with activated carbon as the negative electrode had a specific capacitance of 122.4 F g −1 at 1 A g −1 , a cycling retention rate of 73.53% after 5000 cycles at 5 A g −1 , and a very high energy density of 49.13 Wh kg −1 at power density of 1734.0 W kg −1 . The significantly improved electrochemical performance of the ZnCo-PBA@α-Co(OH) 2 nanocomposites can be attributed to the positive synergistic effects of the porous structure of the PBA material and the large specific surface area of the α-Co(OH) 2 nanosheets, on the ion permeability and number of active sites in the reinforcing material; thus, this composite is a potential material for use in future energy storage systems.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Haotian Hao,Yao Zhang,Shuo Xu,Zihao Wang,Yili Wang,Shan Wang,Baoyou Shi
Enriching low-concentration phosphorus in water is prerequisite for phosphorus recovery. In this study, a polyvinyl alcohol (PVA)-assisted high-temperature stabilization method was developed to synthesize a magnetically recoverable La(OH) 3 -Fe 2 O 3 composite, designated as PMLH, via stable crosslinking. Compared with MLH-1, a conventionally synthesized La(OH) 3 /Fe 2 O 3 composite, PMLH-1 (La/Fe molar ratio = 1:1) exhibited 31.77 % more La(OH) 3 adsorption sites and maintained 2.32 times higher phosphate adsorption capacity after 10 reuse cycles. The optimal synthesis conditions were determined as calcination temperature of 150 °C, PVA dosage of 0.375 %, and La-to-Fe molar ratio of 1.5. Structural characterization revealed that PMLH-1.5 consisted of rod-like La(OH) 3 and irregular γ-Fe 2 O 3 tightly bonded via PVA bridging. The composite demonstrated a maximum phosphate adsorption capacity of 79.51 mg P/g, reaching equilibrium within 16 h at 0.5 g/L dosage. The saturated adsorption remained stable across pH 3–9. While coexisting NO 3 − and humic acid showed negligible effects, Mg 2+ , Cl − , SO 4 2− and HCO 3 − reduced adsorption by 10–20 %, whereas Ca 2+ significantly enhanced phosphate uptake. Notably, PMLH-1.5 exhibited exceptional practical performance, exceeding its theoretical saturation capacity by 20 % with prolonged adsorption in real water matrices. Efficient desorption (4 h) was achieved using 2.5 M NaOH/1.875 M NaCl mixed solution. The PMLH-1.5 demonstrated remarkable stability across 40 consecutive adsorption-desorption cycles using actual water samples, consistently meeting discharge standards for 13–14 full cycles. This performance established a new reference point for cyclic durability assessments in water treatment research. Sequential desorption in the same desorbent progressively concentrated phosphorus from 0 to 26.69 mg/L, enabling effective low-concentration phosphate enrichment. Economic analysis confirmed that PMLH-1.5 exhibits a competitive chemical cost, ranging from 3.28 to 5.26 CNY/mol P (0.46 to 0.74 US $/mol P).
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