CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Shusheng Li,Rui Kuang,Xiangzheng Kong,Xiaoli Zhu,Xubao Jiang
Highly efficient and robust electrocatalysts have been in urgent demand for oxygen evolution reaction (OER). For this purpose, high-cost carbon materials , such as graphene and carbon nanotubes , have been used as supports to metal oxides to enhance their catalytic activity . We report here a new Co 3 O 4 -based catalyst with nitrogen-doped porous carbon material as the support, prepared by pyrolysis of porous polyurea (PU) with Co(NO 3 ) 2 immobilized on its surface. To this end, PU was first synthesized, without any additive, through a very simple one-step precipitation polymerization of toluene diisocyanate in a binary mixture of H 2 O-acetone at room temperature . By immersing PU in an aqueous solution of Co(NO 3 ) 2 at room temperature, a cobalt coordinated polymer composite , Co(NO 3 ) 2 /PU, was obtained, which was heated at 500 °C in air for 2 h to get a hybrid, Co 3 O 4 /NC, consisting of Co 3 O 4 nanocrystals and sp 2 -hybridized N-doped carbon. Using this Co 3 O 4 /NC as a catalyst in OER, a current density of 10 mA·cm −2 was readily achieved with a low overpotential of 293 mV with a Tafel slope of 87 mV·dec −1 , a high catalytic activity. This high performance was well retained after 1000 recycled uses, demonstrating its good durability. This work provides therefore a facile yet simple pathway to fabrication of a new transition metal oxides-based N-doped carbon catalyst for OER with high performance.
研究领域:
材料科学
·
电化学
·
催化化学
·
能源材料
·
纳米科技
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DOI
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
·
2013
·
IF 2.404
Xuan Zhang,Feng Gao,Xili Cai,Meixia Zheng,Fei Gao,Shulian Jiang,Qingxiang Wang
A stable and uniform organic–inorganic nanocomposite that consists of graphene (GR) and pyrenebutyric acid (PBA) was obtained by ultrasonication, which was characterized by scanning electron microscopy (SEM) and UV–vis absorption spectra. The dispersion was dropped onto a gold electrode surface to obtain GR–PBA modified electrode (GR–PBA/Au). Electrochemical behaviors of the modified electrode were characterized by cyclic voltammetry and electrochemical impedance spectroscopy using [Fe(CN) 6 ] 3 −/4 − as the electroactive probe. A novel DNA biosensor was constructed based on the covalent coupling of amino modified oligonucleotides with the carboxylic group on PBA. By using methylene blue (MB) as a redox-active hybridization indicator, the biosensor was applied to electrochemically detect the complementary sequence, and the results suggested that the peak currents of MB showed a good linear relationship with the logarithm values of target DNA concentrations in the range from 1.0 × 10 − 15 to 5.0 × 10 − 12 M with a detection limit of 3.8 × 10 − 16 M. The selectivity experiment also showed that the biosensor can well distinguish the target DNA from the non-complementary sequences.
研究领域:
分析化学
·
生物传感器
·
纳米医学
·
分子诊断
·
电化学
·
基因检测
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高影响因子
Small
·
2022
·Vol. 18
·期 38
·2203693
·
IF 15.153
Tao Zhu,Dongli Chen,Guoqing Liu,Peng Qi,Xiaoyu Gu,Hongfei Li,Jun Sun,Sheng Zhang
Lithium–sulfur batteries (LSBs) have attracted extensive attention owing to their high energy density and abundant sulfur resources. However, LSBs are still restricted by the unsatisfactory electrochemical performance resulting from the shuttle effect of lithium polysulfide (LiPSs), and the potential fire hazard caused by inflammable ether electrolytes and polyolefin separators. Herein, a facile immobilization strategy for hexachlorocyclotriphosphazene (HCCP) is creatively applied to address the above issues simultaneously. Insoluble HCCP cross-linked microspheres (H-CMP) are firstly obtained at ambient temperature using tannic acid (TA) as a cross-linking agent and then a multifunctional separator coating is constructed based on H-CMP. The released phosphorus-related radicals from H-CMP in wide temperatures effectively prevent the combustion of electrolytes and separators, and hence improve the fire safety of the Li–S pouch cell. Furthermore, H-CMP availably chemisorbs LiPSs to interdict the shuttle effect, thereby dramatically improving the electrochemical performance of LSBs. The effectiveness of this strategy is also verified in high sulfur loading (6.38 mg cm -2 ), high temperature (50 °C), and Li–S pouch cells. More importantly, H-CMP exhibits sufficient stability for Li metal and suppression of Li dendrites. This facile immobilization strategy for multifunctional phosphazenes provides a competitive option for the large-scale fabrication of high-safety and high-performance LSBs.
研究领域:
材料科学
·
能源存储技术
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高影响因子
JOURNAL OF NUCLEAR MATERIALS
·
2026
·
IF 3.3
Pengju Chen,Fuhua Xu,Xuchen Yang,Hao Zhang,Tian Tian,Xiangbiao Yin
Nanograin Gd 2 Hf x Zr 2- x O 7 (GHZO, 0.0 ≤ x ≤ 2.0) ceramic was first designed for use as a matrix for immobilizing radionuclides. • The optimal hafnium content ( x Hf ) in GHZO (0.0 ≤ x ≤ 2.0) ceramic was studied and revealed. • Hf-doping can significantly improve the mechanical properties and aqueous corrosion resistance of Gd 2 Zr 2 O 7 material. • The study provides new guidance for the design of HLW curing material with high-performance and environmentally friendliness. A series of novel nanograined Gd₂Hf ₓ Zr₂₋ ₓ O₇ (GHZO, 0.0 ≤ x ≤ 2.0) ceramic samples, designed for nuclear-waste immobilization, were successfully fabricated in this study. The microstructural features, phase evolution, and aqueous corrosion resistance of these samples were thoroughly studied. Results indicated that the GHZO samples (0.0 ≤ x ≤ 2.0) crystallized into a pyrochlore-type structure. As the Hf proportion ( x Hf ) increased from 0.0 to 2.0, the average grain sizes of the GHZO samples remained relatively stable, ranging from 260 to 280 nm. Their relative densities also remained between 95 % and 96 %. The hardness of the GHZO-1.0 sample reached 21.08 GPa, which was significantly higher than that of the GZO (7.91 GPa) and GHO (10.61 GPa) samples. The leaching rates ( LR ) of Zr and Hf in the GHZO-1.0 sample were 1.0 × 10⁻⁷ and 6.8 × 10⁻⁸ g·m⁻²·d⁻¹, respectively, after 42 days of leaching. These values were notably lower than the Zr leaching rate of the GZO sample (8.0 × 10⁻⁷ g·m⁻²·d⁻¹) and Hf leaching rate of the GHO sample (2.9 × 10⁻⁷ g·m⁻²·d⁻¹). This enhanced aqueous durability could be attributed to the higher configurational mixing entropy and lattice distortion. A series of novel nanograin Gd 2 Hf x Zr 2- x O 7 (GHZO, 0.0 ≤ x ≤ 2.0) ceramic samples designed as a nuclear waste forms, were successfully fabricated. The microstructure features, phase transition behavior, and aqueous corrosion resistance were systematically investigated. After 42 days test, the normalized release rates of Zr and Hf elements in the GHZO-1.0 specimen were 1.0 × 10 −7 and 6.8 × 10 −8 g ·m −2 ·d −1 , respectively, much lower than the LR Zr of GZO specimen (8.0 × 10 −7 g ·m −2 ·d −1 ) and LR Hf of GHO specimen (2.9 × 10 −7 g ·m −2 ·d −1 ) owing to the increase of mixed entropy and lattice distortion, exhibiting excellent aqueous durability. The study provides new guidance for the design of HLW curing material with high-performance and environmentally friendly. Download: Download high-res image (393KB) Download: Download full-size image
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LANGMUIR
·
2026
·
IF 4.4
Zhao Yujing,Zhang Xiaowen,Liao Dandan,Qin Dekang,Huang Liyan,Cai Tao,Peng Ying,Chen Zhaowen,Hua Yilong,Wu Xiaoyan,Li Mi
Incorporating Fe 0 into
the porosity of silicon-based
materials can overcome the shortcomings of nanozero-valent iron (nZVI),
such as aggregation, passivation, and secondary release of reduction
products. The mass transfer resistance due to iron oxidation expansion
and consequent pore blockage during uranium reductive coprecipitation
remains unclear. The present work employed amino-functionalized mesoporous
silica (NH 2 –SGB) as the support to precisely regulate
the spatial occupancy rate of Fe 0 in the pores, and synthesized
a series of Fe 0 @NH 2 –SGB ( x -PV, x = 0.00, 0.33, 0.50, and 0.67) composites.
Batch experiments and structural characterization results illustrated
that Fe 0 @NH 2 –SGB (0.33-PV) achieved 97.0%
U(VI) removal and an equilibrium immobilization capacity of 48.3 mg·g –1 from 10 mg·L –1 initial U(VI)
solution at pH 5.0 with 0.2 g·L –1 added, and
a Langmuir-fitted theoretical maximum adsorption capacity of 449.43
mg·g –1 at room temperature, which is better
than that of 0.50-PV and 0.67-PV. The reserved redundant pore of Fe 0 @NH 2 –SGB (0.33-PV) can effectively accommodate
the iron–uranium coprecipitation products, maintain the unobstructed
mass transfer channels, and avoid the orifice blockage effect, resulting
in an effective utilization rate of Fe 0 to 98.2%, which
exceeded that of 0.67-PV (46.7%), the uranium fixation product achieved
a spatial fit of up to 89.1% pore volume and realized confined encapsulation
in the pore. Mechanistic analysis revealed that the immobilization
of U(VI) first took place on the surface of the sample via selective
trapping by −NH 2 groups. Subsequently, the Fe 0 and Fe(II) in the pores efficiently reduced U(VI) to U(IV)
and achieved stable self-sealing immobilization. Meanwhile, continuous
30-day static desorption tests and acid stress tests showed uranium
leaching rates consistently below 0.5%, confirming the long-term stabilization
effect of the confinement encapsulation strategy. It provides a novel
material design strategy for the rational design of confined nanomaterials
and the long-term immobilization of uranium in contaminated groundwater.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Bin Wang,Chuang He,Qiqi Zheng,Li Cao,Shaoyi Wang,Haijie He,Kai Cui,Wenjie Zhang
Heavy metal contamination in soils poses serious threats to the environment and human health. Cement-based solidification/stabilization (S/S) is a common method for treating heavy metal-contaminated soils due to its simplicity and effectiveness. However, the immobilization efficiency of conventional cement systems is limited. In this study, low-cost and highly dispersible novel carbon nanodots (CNDs) are synthesized from citric acid and urea by a microwave-assisted method and added to cement systems to improve the immobilization of Pb and Cd. Leaching results show that, with 15 wt.% cement, the addition of 0.4 wt.% (by weight of cement) CNDs reduces the leaching concentrations of Pb and Cd by 77.3% and 71.8%, respectively. Leaching results and Tessier analyses show that CNDs promote the transformation of Pb and Cd from exchangeable to stable forms and improve chemical stability. XRD, FTIR, DTG, and SEM results show that CNDs accelerate cement hydration and promote the formation of C–S–H gels, which enhances physical encapsulation. FTIR, UV-Vis, and adsorption results further indicate that oxygen- and nitrogen-containing groups on CNDs complex with Pb 2+ and Cd 2+ and strengthen chemical immobilization. This study provides a cost-effective nanomaterial for improving the immobilization of Pb and Cd in cement-based systems and offers new directions for the application of CNDs in sustainable environmental materials.
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PubMed
高影响因子
MOLECULES
·
2026
·Vol. 31
·期 10
·1675
·
IF 5.1
Zixuan Li,Fengyuan Zhang,Shaolei Zhao,Mingbo Sun,Jingru Liu,Yan Xie,Shucai Zhang
Plastic pollution caused by poly(ethylene terephthalate) (PET) highlights the urgent need for efficient biodegradation strategies. However, PET hydrolases such as DuraPETase typically exhibit limited substrate affinity for PET and insufficient operational stability. Although conventional immobilization improves enzyme stability, it often compromises catalytic activity. Here, we design a PET-targeting, orientation-controlled immobilization strategy that overcomes this traditional trade-off and enables efficient PET biodegradation. Guided by rational structural analysis, three Cys variants (R53C, R59C, R224C) were engineered for site-specific covalent attachment to a PDA@SiO2support with inherent PET-binding capability. The resulting conjugates (DuraR53C-PDA@SiO2, DuraR59C-PDA@SiO2, and DuraR224C-PDA@SiO2) displayed distinct catalytic and stability profiles. Among them, DuraR59C-PDA@SiO2achieved the optimal balance between activity and stability, retaining kinetic properties comparable to the free enzyme and maintaining 87.6% residual activity after 2 h at 80 °C. Water contact angle measurements confirmed its PET-targeting behavior, as evidenced by the reduction in the PET contact angle from 85° to 45°. In 10-day degradation assays at 50 °C, DuraR59C-PDA@SiO2released a total of 4865.32 μM degradation products, representing a 2.37-fold increase relative to free DuraPETase. These findings demonstrate an effective strategy for industrial enzymatic PET degradation and recycling.
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高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2026
·
IF 3.9
Nan Wang,Xingsheng Liu,Pen Jin,Zirui Guo,Jianxin Xu,Zhenbin Chen
The catalytic performance of tyrosinase (TYR) is highly sensitive to its microenvironment, which poses challenges for its application in immobilized systems. Here, we systematically investigated the effects of different liquid-phase environments (organic solvents and ions) on TYR activity using molecular dynamics (MD) simulations and experimental assays. The results showed that TYR maintained its overall structural integrity in all tested environments, whereas its catalytic activity varied considerably. Global structural parameters ( RMSD , Rg , SASA ) reflected solvent-induced conformational changes and showed correlations with activity variations. Further analysis of local dynamics via RMSF , secondary structure ( DSSP ), and the coordination geometry of the Cu 2 + -histidine catalytic center suggested that increased flexibility near the catalytic pocket might be associated with activity loss. Based on these findings, solvents that minimize local flexibility changes and avoid direct interaction with the catalytic center are considered preferable for preserving activity. Moreover, we propose a carrier design consisting of an Fe 3 O 4 magnetic core coated with highly chlorinated polyvinyl chloride (CPVC), with Cu 2+ incorporated during coating to potentially help maintain active-site integrity. This work provides preliminary insights into the relationship between microenvironment, structural dynamics, and enzyme activity, and offers guidance for solvent selection and the design of immobilized enzyme systems.
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高影响因子
BIOELECTROCHEMISTRY
·
2026
·
IF 4.9
Jintian Zhang,Feixuan Li,Xiaoyan Xiang,Xinxin Xiao,Shizhen Wang
Deep eutectic solvents (DESs) are a group of emerging solvents for biocatalysis with tailored performance. Herein, we report the usage of hierarchical zeolitic imidazole framework-8 (HZIF-8) and halogenated DES for the immobilization of phenylalanine dehydrogenase. Effects of three different halogenated DESs (I, Cl and Br) on the activity of immobilized enzymes for production of homophenylalanine were studied. The optimal activity towards with the model reaction of catalyzing ethyl 2-oxo-4-phenylbutyrate (EOPB) to L -homophenylalanine was 6.11 U/mg at 70 °C, 5.4-fold of that of the free enzyme, with 78.4% of its original activity retained after six recycles. The immobilized enzymes were further loaded on a poly(methylene blue) electrode with electrochemical NAD + regeneration, leading to bioelectrosynthesis of phenylpyruvate. Using phenylalanine-ethanolamine (Phe-MEA) as the substrate, 13.85 mM phenylpyruvate was obtained after 8 h, with a total turnover number (TTN) value of 138.5 for NADH regeneration, while a TTN of 102.2 using L-Phe as the substrate.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2026
·
IF 8.7
Weiguo Wu,Ran Gao,Mingyue Wu,Ting Sun,Xijun Hao,Chongyang Hu,Yikang Shu,Danhua Li,Shuai Ji
Immobilized kinases are capable of catalyzing the in vitro phosphorylation of substrates, offering the advantages of recoverability and reusability. Nevertheless, existing immobilization strategies are often limited by intricate procedures and suboptimal biocompatibility. In this work, we selected Akt (protein kinase B) as a model enzyme and developed an efficient immobilization strategy based on a magnetic aldehyde-functionalized ionic liquid support. Key advantages of this approach include a short immobilization time, avoidance of toxic crosslinkers, and applicability to protein-level phosphorylation. A dual-aldehyde-functionalized ionic liquid was synthesized using 4-(imidazol-1-yl)benzaldehyde as the cation and 3-bromo-4-aldehyde-benzoic acid as the anion. This ionic liquid was anchored onto Fe 3 O 4 to yield the novel magnetic nanocomposite Fe 3 O 4 @SiO 2 @[ImBa][BABa], which was characterized by SEM, TEM, IR, EDS, TGA and VSM analyses. Akt was immobilized onto this carrier via Schiff base covalent linkage between aldehyde and amino groups. The optimal immobilization parameters were identified, and the immobilized Akt exhibited enhanced catalytic activity relative to conventional immobilization approaches. Furthermore, the immobilized enzyme demonstrated superior substrate affinity and storage stability compared with its free counterpart, as well as proof-of-concept reusability over four cycles (>80% residual activity). Importantly, the immobilized Akt retained its ability to catalyze the phosphorylation of both peptide and protein (GSK3β) substrates, underscoring its practical potential. To the best of our knowledge, this study represents the first application of magnetic ionic liquids for kinase immobilization and the first establishment of an immobilization protocol for Akt.
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Yueru Fang,Zhiqiang Guo,Tanveer Hussain,Xiaoyong Lv,Ronghua Li
Organoarsenical contaminants such as roxarsone (ROX) pose a persistent challenge in water treatment because oxidative degradation of the parent compound inevitably generates inorganic arsenic (iAs), whereas adsorption-based processes immobilize iAs without removing the organoarsenical precursor. As a result, arsenic is redistributed among species rather than eliminated, and its overall fate during transformation and immobilization remains poorly quantified. Here, we develop a Co-doped LaOCl catalyst (Co 0.5 LOC) that enables coupled oxidative transformation and arsenic immobilization under peroxymonosulfate (PMS) activation via spatially integrated Co and La sites. Critically, a complete time-resolved arsenic mass balance is achieved throughout the reaction, with total arsenic recovery maintained at 100 ± 2%, thereby directly linking ROX degradation, iAs formation, and final immobilization. The catalyst exhibits a pseudo-first-order ROX degradation rate of 0.2935 min −1 , 2.2-fold higher than pristine LaOCl, with >96% removal across pH 5–9 and >81% activity retention after five cycles. Mechanistic analysis identifies surface-confined singlet oxygen ( 1 O 2 ) as the dominant reactive species, providing strong resistance to chloride ions and natural organic matter. A synergy index of 6.72 quantifies non-additive oxidation–adsorption coupling. Total organic carbon monitoring reveals that structural transformation substantially exceeds mineralization, with approximately 26% of the initial carbon remaining at 120 min; LC-HRMS tentatively identifies four aromatic intermediates in the residual fraction, consistent with the limited ring-opening capability of surface-confined 1 O 2 . Overall, this work establishes a unified strategy for organoarsenic remediation by integrating oxidative destruction with quantitative arsenic sequestration, enabling comprehensive contaminant fate accountability in advanced water treatment systems.
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高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Huihui Liu,Yihan Liu,Zhongmu Han,Yufei Zhang,Mingming Zheng
Phosphatidylserine (PS) is a high-value phospholipid in functional foods and pharmaceuticals. However, the lack of a suitable biocatalytic system has limited the conversion efficiency. A novel Pickering interfacial biocatalysis (PIB) system has developed for converting phosphatidylcholine (PC) to PS in this work. Three immobilized enzyme carriers were synthesized by grafting different modifying groups onto hollow mesoporous silica particles (HMSP). The combination of NQ-62 and octyl-modified groups yielded the optimal immobilized enzyme, PLD@HMSP-N 3 /C 8 . It stabilized the water-in-oil Pickering emulsion and enhanced phospholipase D (PLD) stability via hydrogen bond interactions. Under optimized conditions, a PS conversion of 93.8 % was achieved within 20 min at 40 °C, achieving a catalytic efficiency (CE) of 372 mmol/(g·h). The immobilized PLD demonstrated markedly enhanced thermostability, pH resistance, and protease hydrolysis stability compared to its free and homologous series counterparts. Moreover, it retained 70.9 % of the PS conversion after 10 cycles of reuse.
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高影响因子
危险品化学品经营许可证（带存储）