JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Rajapriya Andavar,Mameng Yang,Cunpeng Duan,Anuj Kumar,Yanzhi Sun,Junqing Pan
Industrial-level alkaline water electrolysis requires high-efficiency catalysts to achieve rapid water dissociation and hydrogen intermediate migration at an ampere-level current density. However, conventional alloy catalysts lack spatially organized, abundant site functions, resulting in poor coupling between alkaline electrolysis steps. Here, we report a new NiCoFeCuMoW high-entropy alloy (HEA) catalyst prepared by pulse electrodeposition, featuring efficient mass and charge transport. The catalyst features a three-dimensional hierarchically porous framework with tailored surface atomic configurations and chemically differentiated multimetallic motifs, enabling abundant accessible active sites, accelerated transport, and cooperative regulation of reaction intermediates. Density functional theory (DFT) calculations show that Mo/W-richdomains preferentially facilitate H 2 O dissociation, whereas adjacent NiCoFeCuMoW ensembles optimize hydrogen diffusion and intermediate stabilization via regulated d-band states, thereby establishing an efficient dissociation-diffusion cascade. The NiCoFeCuMoW HEA delivers overpotentials of only 36 mV within the hydrogen evolution reaction (HER) while exhibiting 226 mV in the oxygen evolution reaction (OER) operating in alkaline electrolytes at 10 mA cm −2 . Amazingly, the cell delivers an ultra-low electrolyte potential of 1.57 V at 120 °C and 1 A cm −2 , owing to greatly enhanced charge-mass transport and perturbed hydrogen-bond networks in the over-boiling environment, providing a scalable HEA design strategy for ampere-level industrial water splitting. The boosted electrocatalytic acitivity of new HEAs alloy catalyst under over-boiling environment. Download: Download high-res image (204KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shucheng Liu,Ying Sun,Danzhao Guo,Ruiheng Lu,Yuying Mao,Hongxiang Ou
For porous molecular imprinted polymers (MIPs), introduction of special functional groups and integration porous structure support will endow the MIPs with tunable surface properties and specific affinity performance. Herein, by combination of RAFT molecular imprinting, Pickering emulsion, and boronate affinity methods, a new kind of porous imprinted microspheres (BA-HPMIPs) using the low pKa value of APBA (1-allylpyridinium-3-boronic acid, pKa = 7.4) as functional monomer was prepared for specific molecular recognition and separation of NRG. Meanwhile, the novel RAFT functioned surfactants with dual amide multiple H-bonds were designed as stabilized particles was used to promote sustainability, which further confer them multifunctionality and/or by polymerizing the Pickering emulsion itself. Equilibrium adsorption was reached rapidly within 360 min, and the maximum equilibrium binding capacities of BA-HPMIPs were found to be 118.32 µmol g −1 for NRG. Furthermore, they had a stronger selectivity towards NRG than other competitive target (i.e rutin, catechol, ARS, o -nitrophenol). Moreover, BA-HPMIPs have shown outstanding reusability of 8.63 % loss in enrichment performance after five times repeatedly. As a proof of this concept, a commercially avaliable NRG with purity could be effectively extracted and concentrated to 96.75 % purity. These results demonstrated that, a new kind of porous imprinted microsphere with abundant porous structure and boronic acid recognizing sites has great potential for separation and purification of industrial samples under neutral conditions.
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JOURNAL OF BIOSCIENCE AND BIOENGINEERING
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2019
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IF 2.032
Xiaohong Lu,Juhua Chen,Linshu Jiao,Lei Zhong,Zhaoxin Lu,Chong Zhang,Fengxia Lu
Directed evolution methodologies have been used as promising strategies for improving the catalytic properties of many existing enzymes . In the presented work, this approach was applied to improve the enzyme activity of l -asparaginase I obtained from Bacillus megaterium H-1. After two rounds of error-prone polymerase chain reaction (epPCR) and two generations of sequential DNA shuffling , all of 5 different mutants showed a significant increase in the enzyme activity of l -asparaginase I, ranging from 6.27 to 22.78 IU/mL. Among these mutants, D-9B and DD-12G displayed the relatively high catalytic activity , which were 20.22-fold and 21.33-fold higher than the wild-type enzyme (WT), respectively. Furthermore, the catalytic efficiency ( k cat / K m ) of D-9B and DD-12G were also improved, which were 132.73 min −1 mM −1 and 146.39 min −1 mM −1 , respectively, in comparison to that of WT (3.39 min −1 mM −1 ). In addition, mutant DD-12G showed tolerance toward wider range of pH values and higher temperatures than its WT counterpart. Homology modeling of above two mutants reflected a reduction of hydrogen bonds and an introduction of flexible residues in the loops near the active catalytic site Thr15. These changes contributed to the flexibility of loops, which may lead to further enhancement in catalytic efficiency. Results also showed that approximately 88.5% (0.978 mg/kg) acrylamide could be removed from mutant DD-12G pre-treated fried potato chips. This study clearly shows that directional evolution methods can indeed be utilized to improve the activity of l -asparaginase, which could also provide research basis for future application in food industry.
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DALTON TRANSACTIONS
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2014
·Vol. 43
·期 24
·9216-9225
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IF 4.097
Qiong Wu,Tianfeng Chen,Zhao Zhang,Siyan Liao,Xiaohui Wu,Jian Wu,Wenjie Mei,Yanhua Chen,Weili Wu,Lingli Zeng,Wenjie Zheng
Two arene Ru(II) complexes coordinated by 2-(3-methoxyphenyl)imidazole[4,5-f][1,10]phenanthroline, [(η6-RC6H5)Ru(m-MOPIP)Cl]Cl (R = H, 1; R = CH3, 2), have been prepared under microwave irradiation; the crystal structure of 2 exhibits a typical “piano stool” conformation, with bond angles for N1–Ru1–Cl1 86.02 (14)° and N2–Ru1–Cl1 84.51 (14)°. The Ru–C distance for the Ru atom bound to the benzene ring is about 0.2178(8) nm, and the average Ru–N distance for Ru atom to the two chelating N atoms is about 0.2092(4) nm. The evaluation of in vitro anticancer activities revealed that these synthetic Ru(II) complexes selectively inhibited the growth of HepG2 hepatocellular carcinoma cells, with low cytotoxicity toward LO2 human normal liver cells. The results demonstrated that the complexes exhibited great selectivity between human cancer and normal cells by comparing with the ligand m-MOPIP. Furthermore, complexes 1 and 2 could bind to c-myc G4 DNA in groove binding mode in promising affinity, and the insertion of the methyl groups in the arene ligand contributed to strengthen the binding affinity. This was also confirmed by molecular docking calculation and 1H NMR analysis which showed that both 1 and 2 can bind in the loop constructed by A6–G9 and G21–A25 base pairs in c-myc G4 DNA to block the replication of c-myc oligomer. Taken together, these results suggest that arene Ru(II) complexes display application potential as small molecule inhibitors of c-myc G4 DNA.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Huiqin Ma,Weiyi Yang,Shuang Gao,Zifeng Lin,Zheyang Mo,Chao Li,Jian Ku Shang,Qi Li
Recently, photoassisted charging has been demonstrated as a green and sustainable approach to successfully enhance the capacitance of supercapacitors with low cost and good efficiency. However, their light-induced capacitance enhancement is relatively low and is lost quickly when the illumination is off. In this work, a novel active material system is developed for supercapacitors with the photoassisted charging capability by the decoration of a small amount of Bi2WO6 nanoparticles on an h-WO3 submicron rod surface in situ, which forms a typical type II band alignment heterostructure with a close contact interface through the co-sharing of W atoms between h-WO3 submicron rods and Bi2WO6 nanoparticles. The photogenerated charge carrier separation and transfer are largely enhanced in the h-WO3/Bi2WO6 submicron rod electrode, which subsequently allows more charge carriers to participate in its photoassisted charging process to largely enhance its capacitance improvement under simulated solar illumination than that of the h-WO3 submicron rod electrode. Furthermore, the h-WO3/Bi2WO6 submicron rod electrode could retain its photoinduced capacitance enhancement in the dark for an extended period of time from the photocatalytic memory effect. Thus, our work provides a solution to the two major drawbacks of reported supercapacitors with the light-induced capacitance enhancement property, and supercapacitors based on active materials with the photocatalytic memory effect could be utilized in various technical fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Kok Bing Tan,Pan Tian,Xinxin Zhang,Jian Tian,Guowu Zhan,Jiale Huang,Qingbiao Li
The present study developed bifunctional catalyst for CO 2 hydrogenation into dimethyl ether (DME), whereby it consists of Pd/In 2 O 3 for CO 2 hydrogenation into methanol, and H-ZSM-5 for methanol dehydration into DME. The catalyst development was focused on the synthesis of Pd/In 2 O 3 via a green and low-cost synthesis method of carbonized alginate templating. Thus, microspherical-confined nano-Pd/In 2 O 3 was formed, whereby the localized nucleation growth was coordinated by the chemically entrapped In 3+ via ionic bond in the well-distributed alginate structure. It was found that hydrothermal temperature plays a key role in the development of this catalyst structure. The optimum hydrothermal temperature is 160 °C, as it is able to produce the highest amount of methanol. This catalyst was further integrated with H-ZSM-5 via different integration manners. It was found that mortar mixed method produces the highest amount of DME, as the close proximity causes stronger ion-exchange mechanism between the catalyst components, which facilitates higher oxygen vacancy density in the bifunctional catalyst. Under the optimum Pd/In 2 O 3 : H-ZSM-5 (PdIn-160–12: H-ZSM-5) mass ratio of 4:1, the highest STY DME of 79.7 g DME kg cat -1 h −1 with CO 2 conversion of 9% and DME selectivity of 44.1% can be achieved. In addition, the STY DME can be maintained even in 60 h on stream, demonstrating the excellent stability and performance of microspherical-confined nano-Pd/In 2 O 3 /H-ZSM-5 bifunctional catalyst synthesized via carbonized alginate templating strategy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Xu Huang,Xuezhang Xiao,Xuancheng Wang,Zhendong Yao,Jiahuan He,Xiulin Fan,Lixin Chen
Li–Mg–B–H reactive hydride composite (RHC) has attracted extensive attention over the past decades for its extremely high hydrogen storage capacity (11.5 wt%). But the sluggish desorption kinetics for the second step dehydrogenation reaction need to be further improved. Herein, short rod-like TMTiO 3 (TM = Co, Ni) bimetallic oxides , which contain two kinds of transition metal elements, were synthesized and introduced into Li–Mg–B–H RHC for the first time. The NiTiO 3 exhibits excellent catalytic effect on the hydrogen desorption kinetic performance of Li–Mg–B–H RHC, and the incubation period for the second step dehydrogenation reaction is eliminated completely by reducing the apparent activation energy for the generation of MgB 2 from 296 kJ/mol to 269 kJ/mol. The NiTiO 3 doped Li–Mg–B–H RHC can desorb about 9.0 wt% H 2 without obvious attenuation of kinetic performance in five cycles. Mechanism analyses reveal that the in-situ generated nano-sized MgNi 3 B 2 and TiB 2 species (∼5 nm) both meet the critical value ( < 10%) of the edge-to-edge matching model (5.77% for MgNi 3 B 2 and 2.22% for TiB 2 ), which play a significant role in supporting the nucleation of MgB 2 . Meanwhile, the extremely fine MgNi 3 B 2 and TiB 2 heterogeneous nucleation sites can inhibit the excessive growth for a single crystal nucleus of MgB 2 . The heterogeneous nucleation and grain refinement mechanisms caused by the novel bimetallic oxide could provide alternative insights into designing an in-situ generated nano-sized catalytic hydrogen storage system with enhanced kinetics and cyclic stability for hydrogen-fueled applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
·
IF 9.6
Siqi Liu,Shanshan Cheng,Zhimeng Liu,Miaomiao Zheng,Hongyuan Wang,Supakorn Boonyuen,Hongyi Gao,Ge Wang
Reactive oxygen species (ROS)-mediated sterilization typically relies on continuous light irradiation or exogenous H 2 O 2 addition, limiting their practical utility under dark or resource-limited conditions. Herein, we rationally design an S-scheme MIL-100(Fe)/Zn 3 In 2 S 6 heterojunction (M 5 Z 1 –1@ZIS2) by in-situ growing Zn-doped MIL-100(Fe) on Zn 3 In 2 S 6 , achieving synergistic light-harvesting and ROS self-supply capabilities. The incorporation of Zn 3 In 2 S 6 enhances electron density around Fe 2+ sites while modulating Fe 3+ states, significantly improving O₂ activation and H 2 O 2 affinity. This unique electronic regulation enables the heterojunction to generate superoxide radical(·O₂ − )-dominated ROS even in the dark. Notably, visible-light pretreatment induces active In sites in Zn 3 In 2 S 6 to produce H 2 O 2 , which accumulates and sustains the FeII/FeIII redox cycle in the absence of light, driving continuous hydroxyl radical(·OH)-dominated ROS generation. Combined characterizations including X-ray photoelectron spectroscopy (XPS) and Electron Paramagnetic Resonance (EPR) confirm H₂O₂-mediated Fe 2+ regeneration and ROS persistence. The M 5 Z 1 –1@ZIS2 heterojunction exhibits exceptional antibacterial performance, achieving ≥99.9% inactivation of Escherichia coli ( E. coli ) within 1.5 h in the dark and 40 min under visible light. This work provides a strategy for designing self-sustaining catalytic systems that leverage light-driven H₂O₂ supply to enable day-night ROS functionality. Furthermore, M 5 Z 1 –1@ZIS2 loaded on polyvinylidene fluoride (PVDF) film can achieve an efficiency of over 99% for particulate matter (PM) pollutants at the wind speeds of 1.5 m/s and 0.5 m/s and reach a maximum adsorption efficiency of 99.5% for formaldehyde within 19 min, highlighting its potential for all-weather air purification via ROS-mediated environmental remediation.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2019
·
IF 3.714
He Li,Xiang-Yi Tang,Chun-Jian Wu,Shu-Juan Yu
The 2,3-dihydro-3,5-dihydroxy-6-methyl-4(H)-pyran-4-one (DDMP) is one of the Mallard reaction product with intense bitter and strong antioxidant activity . Insight into DDMP formation pathways is important to manage Maillard reaction products quality. In this work, wet- and dry-heating glucose-amino acid model reactions were investigated to understand the DDMP formation pathways. Lysine and proline facilitated the DDMP generation in wet- and dry-heating system, respectively, suggesting the reaction intensity and amino acid properties are primary factors mediating DDMP generation. Fundamental mechanism on DDMP formation or inhibition was evaluated via quantitatively monitoring enolization products, which suggested that the formation of DDMP was facilitated at lower moisture content condition caused by more 1-deoxyglucosone (1-DG) generation via 2,3-enolization. However, increasing moisture content resulted in the decay of DDMP because of the transformation of 2,3-enolization to 1,2-enolization, which inhibited DDMP generation but transformed to form 5-hydroxymethylfurfural (HMF).
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2019
·
IF 3.571
He Li,Chun-Jian Wu,Xiang-Yi Tang,Shu-Juan Yu
The control of 2,3-dihydro-3,5-dihydroxy-6-methyl-4(H)-pyran-4-one (DDMP) formation in the Maillard reaction is important to improve the thermally treated food quality as a result of its intense bitterness and potential toxicity. In this work, phenolic acids, such as gallic, protocatechuic, caffeic, and ferulic acids, were applied to modulate DDMP formation in a microaqueous glucose–proline model. The formation of DDMP was inhibited at low concentrations (from 0.1 to 5.0 mM) while enhanced at 10.0 mM gallic, protocatechuic, and caffeic acids. Ferulic acid always inhibited DDMP formation as a result of the absence of catechol groups on its benzene ring. The result indicated that the control of DDMP formation depended upon the concentration and chemical structures of phenolic acids, such as the number of hydroxyl groups. Further studies indicated that the hydroxyl distribution of phenolic acids regulated the peroxide formation in the model reaction system and further changed the development of the oxidation reaction, which affected the degradation of glucose via caramel or Maillard reaction, Amadori rearrangement product oxidation, and 1-deoxyglucosone degradation to form the intermediates.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaoyu Wang,Mengchao Feng,Rui Cao,Yuchang Wang,Kai Ma,Jianbin Zhang
A new CeCO 3 OH@(hexagonal/cubic phases–CdS) (CeCO 3 OH@(H/C–CdS)) composite catalyst was facilely synthesized by a simple microinjection titration–stirring method, in which CdS nanoparticles were dispersed on the surface of CeCO 3 OH nanolines. The optimal conditions for the preparation of composite catalysts with high photocatalytic performance were determined by single-factor experiments and response surface experiments. Under these conditions, the degradation rate of 30 mL 2.000 g/L rhodamine B (Rh B) by CeCO 3 OH@(H/C-CdS) in a photocatalytic reaction for 1 h at 25 °C was up to 86.81 % and its degradation rate in a photocatalytic reaction for 150 min was up to 99.62 %. The degradation rate could be maintained above 80 % even after six times recycling. Especially, the photocatalytic degradation efficiency of 2.000 g/L Rh B on the composite catalyst under sunlight and at room temperature for 30 min reached 97.66 %. Meanwhile, the large size of CeCO 3 OH considerably alleviated the agglomeration of CdS, providing more adsorption and active sites for visible light-mediated degradation of Rh B. Importantly, the Z-scheme charge transfer realized by CdS and CeCO 3 OH enhanced the efficient separation of photogenerated electrons and holes, and successfully inhibited the recombination of photogenerated electrons with holes. At the same time, owing to the low energy band difference between the two phases of CdS, charge was transferred between the hexagonal and cubic phases, leaving more effective photogenerated charge to participate in the degradation of Rh B. The synergism of the heterophase junction and heterojunction and the presence of oxygen and sulfur vacancies considerably enhanced the degradation performance of the catalyst. Thus, this study provides a new strategy for the modification and enhanced visible-light catalysis performance of CdS-based catalysts.
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ENERGY & FUELS
·
2024
·
IF 5.2
Ziyi Li,Li Huang,Xiaoyang Yu,Kun Huang,Wenbo Cui,Hong Zhang
The development of stable and efficient ODS catalysts for achieving room-temperature catalytic oxidation desulfurization is one of the challenges in the field of catalytic oxidation desulfurization. This work successfully synthesized and evaluated a new type of composite catalyst, Mo8/h-BN, using the wet impregnation method to investigate its desulfurization performance under various conditions. ODS tests were conducted on DBT, BT, and 4,6-DMDBT using Mo8/h-BN as the catalyst, H2O2 as the oxidant, and [BMIM]PF6 as the extractant. Characterization and testing revealed that Mo8/h-BN exhibited excellent ODS activity, converting DBT completely at 60 °C in 10 min. This study not only explored the optimal desulfurization conditions but also investigated the desulfurization performance of the catalyst at room temperature. Additionally, it is speculated that there may be an electron transfer between Mo8 and h-BN, which enhances the stability of the catalyst. Finally, possible CODS mechanisms were inferred through GC-MS and free radical trapping experiments. In conclusion, the composite catalyst Mo8/h-BN provides a new pathway for developing low-energy consumption, sustainable, cost-effective, and efficient desulfurization catalysts.
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