BIOTECHNOLOGY AND BIOENGINEERING
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2024
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IF 3.5
Han-Yu Liu,Pan Ning,Feng Qian,Yao-Wu Wang,Hai-Min Zhang,Pu Wang
Flavin-dependent halogenase (FDH) is highly prized in pharmaceutical and chemical industries for its exceptional capacity to produce halogenated aromatic compounds with precise regioselectivity. This study has devised a multi-enzyme self-assembly strategy to construct an effective and reliable in vitro coenzyme cycling system tailored for FDHs. Initially, tri-enzyme self-assembling nanoclusters (TESNCs) were developed, comprising glucose dehydrogenase (GDH), flavin reductase (FR) and FDH. The TESNCs exhibited enhanced thermal stability and conversion efficiency compared to free triple enzyme mixtures during the conversion of L -Trp to 6-Cl- L -Trp, resulting in a 2.1-fold increase in yield. Subsequently, an ordered co-immobilization of GDH, FR, and FDH was established, further amplifying the stability and catalytic efficiency of the FDH coenzyme cycle system. Compared to the free TESNCs, the immobilized TESNCs demonstrated a 4.2-fold increase in catalytic efficiency in a 5 mL reaction system. This research provides an effective strategy for developing a robust and efficient coenzyme recycling system for FDHs.
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高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Wei Shengjie,Ma Wenjie,Sun Minmin,Xiang Pan,Tian Ziqi,Mao Lanqun,Gao Lizeng,Li Yadong
Constructing atom-pair engineering and improving the activity of metal single-atom nanozyme (SAzyme) is significant but challenging. Herein, we design the atom-pair engineering of Zn-SA/CNCl SAzyme by simultaneously constructing Zn-N 4 sites as catalytic sites and Zn-N 4 Cl 1 sites as catalytic regulator. The Zn-N 4 Cl 1 catalytic regulators effectively boost the peroxidase-like activities of Zn-N 4 catalytic sites, resulting in a 346-fold, 1496-fold, and 133-fold increase in the maximal reaction velocity, the catalytic constant and the catalytic efficiency, compared to Zn-SA/CN SAzyme without the Zn-N 4 Cl 1 catalytic regulator. The Zn-SA/CNCl SAzyme with excellent peroxidase-like activity effectively inhibits tumor cell growth in vitro and in vivo. The density functional theory (DFT) calculations reveal that the Zn-N 4 Cl 1 catalytic regulators facilitate the adsorption of * H 2 O 2 and re-exposure of Zn-N 4 catalytic sites, and thus improve the reaction rate. This work provides a rational and effective strategy for improving the peroxidase-like activity of metal SAzyme by atom-pair engineering.
研究领域:
材料科学
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催化
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纳米技术
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生物化学
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理论化学
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2026
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IF 2.4
Ziyu Zhuang,Manman Zhang,Dandan Gao,Wolfgang Voigt,Dongdong Li,Haitao Feng
Previously, the formation of a stable adduct 2H3BO3·3CsCl (BC) was observed in CsCl(aq) but not in RbCl(aq). The phase equilibria of the H3BO3 + RbCl + CsCl + H2O system were studied to assess the potential for selective separation of Cs from Rb. Solubility isotherms were determined experimentally. Appropriate liquid composition ranges were preselected using modeling with ISLEC’s equilibrium software. Schreinemakers’ wet solid method, XRD, Raman and IR spectra, Roozeboom’s plots, and SEM-EDS were applied to identify the four phase regions H3BO3, 2H3BO3·3(Cs,Rb)Cl (Bss), (Rb,Cs)Cl, and (Cs,Rb)Cl. Notably, in the presence of RbCl, the BC phase incorporates Rb+, forming a substitutional solid solution, Bss, which inhibits selective separation of CsCl. Roozeboom’s plot analysis revealed that RbCl exhibits higher solubility in the Bss phase compared to the (Cs,Rb)Cl solid solution. The separation factor βCs/Rb between the solid Bss phase and the corresponding solution was 2.0, significantly lower than that of (Cs,Rb)Cl (βCs/Rb = 9.5) in the ternary system without H3BO3. This indicates a stronger coordination between CsCl and H3BO3 relative to that of RbCl in the ternary system without H3BO3. The above understanding provides new strategies designing novel B–OH compounds to enhance Cs/Rb separation efficiency in aqueous systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yong Liu,Yong Chen,Yufeng Da,Fei Xie,Jianlong Wang
Herein, we report an integrated coagulation/ photo-Fenton (CPF) process for advanced treatment of mature landfill leachate using nascent aluminum ions as coagulant and hydrogen peroxide (H 2 O 2 ) as oxidant for Fenton reaction , which were in-situ produced by a novel chlorine and nitrogen co-doped aluminum-graphite (Cl, N-Al-Gr) composite. The coagulation of the MBR-treated landfill leachate was performed by nascent aluminum ions generated in Cl, N-Al-Gr/O 2 system; and the resulting coagulation effluent was treated by photo-Fenton oxidation in the presence of ultraviolet (UVA). The Cl, N-Al-Gr composite exhibited excellent performance for in-situ H 2 O 2 production (813.9 mg/L). The humic substances in landfill leachate could promote the cycle of Fe 3+ /Fe 2+ , and the removal efficiency of total organic carbon (TOC) and color was 88.1% and 97.6%, respectively under the optimized condition. The current study suggested that “coagulation + Fenton” process using nascent Al 3+ as coagulant and in-situ generated H 2 O 2 for Fenton oxidation could be a new way for wastewater treatment .
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2021
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IF 3.178
Yaqi Ding,Neng Gao,Nian Li,Guangming Chen,Yongmei Xuan
The vapour-liquid equilibrium (VLE) data of four ternary solutions HCOOK + [Emim]Ac /[Emim]Br / [Emim]Cl / [Emim]NO 3 + H 2 O were measured using the boiling method at the temperatures from 305.78 K to 387.08 K, at solute (HCOOK + IL) mass fractions ( w ) between 0.2 and 0.5. A total of 234 data points ( w = 0 included) were obtained and correlated with empirical Antoine-type equations. The absolute average relative deviations (AARD %) between calculated and measured vapour pressures were 0.58%, 0.50%, 0.49%, 0.63%, respectively, which showed good agreement. The comparison of the experimental and standard data and combined uncertainties of the experimental data confirmed good reliability of the experimental method and apparatus. The four ternary solutions with ILs as additives have lower vapour pressure compared to the corresponding binary solutions without ILs. The results showed that the four ternary solutions of HCOOK + [Emim]Ac / [Emim]Br / [Emim]Cl / [Emim]NO 3 + H 2 O can be the alternatives for traditional dehumidification and absorption media. [Emim]Cl has the best ability to reduce the vapour pressure of HCOOK + H 2 O at the solute (HCOOK + IL) mass fraction of 0.4 and 0.5. The [Emim]Ac has the most effect reducing the vapour pressure of HCOOK + H 2 O at the solute (HCOOK + IL) mass fraction of 0.3.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2020
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IF 2.888
Zhan-Ping Qiao,Tian Yang,Shu-Zhi Cao,Yu-Feng Tang,Qi-Chao Yang
Solid-liquid equilibria in the ternary systems RbX + CdX 2 + H 2 O (X = Cl, Br) at T = 298.15 K and under 101.3 kPa were investigated by the method of isothermal solution saturation, and the corresponding phase diagrams were constructed. It was found that there were five crystallization regions corresponding to CdCl 2 ·2.5H 2 O, RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 and RbCl in the system (RbCl + CdCl 2 + H 2 O). Four crystallization regions corresponding to CdBr 2 ·4H 2 O, RbCdBr 3 , Rb 4 CdBr 6 and RbBr were found in the system (RbBr + CdBr 2 + H 2 O). The new solid compounds RbCdCl 3 , RbCdBr 3 and Rb 4 CdBr 6 were congruently soluble in water, and new double salts RbCd 2 Cl 5 ·H 2 O and Rb 4 CdCl 6 were incongruently soluble in water. The new solid-phase compounds RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 , RbCdBr 3 and Rb 4 CdBr 6 were characterized by chemical analysis, XRD and TG-DTG techniques. The standard molar enthalpies of solution of RbCd 2 Cl 5 ·H 2 O, RbCdCl 3 , Rb 4 CdCl 6 , RbCdBr 3 and Rb 4 CdBr 6 in water were measured to be (20.74 ± 0.16) kJ·mol −1 , (28.00 ± 0.39) kJ·mol −1 , (96.56 ± 0.50) kJ·mol −1 , (35.38 ± 0.33) kJ·mol −1 and (110.64 ± 0.62) kJ·mol −1 by microcalorimetry in the condition of infinite dilution, and their standard molar enthalpies of formation were determined to be −(1545.3 ± 0.6) kJ·mol −1 , −(856.5 ± 0.7) kJ·mol −1 , −(2180.1 ± 1.3) kJ·mol −1 , −(727.1 ± 0.7) kJ·mol −1 and −(1920.5 ± 1.3) kJ·mol −1 , respectively.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Haitao Zhou,Zhizhuo Yang,Xueqin Wu,Kun Huang
The separation process in hydrochloric acid environments is determined by the interfacial chemistry of the acid. However, the surface species of concentrated acids are complex. The effect of dominant species on the surface of concentrated acids and their dissociation behavior on interfacial separation has been the focus of academic debate. The extraction and separation of two typical anions, PdCl 4 2− and PtCl 6 2− , with different hydration characters on the surface of concentrated hydrochloric acid were investigated by thin layer extraction (TLX). A new phenomenon was discovered that the effect of hydrochloric acid concentration, extractant concentration, organic film thickness, and shear flow rate on the extraction of easily hydrated PdCl 4 2− anions is greater than that of hardly hydrated PtCl 6 2− . However, during the conventional SX process, the phenomenon cannot be observed due to the continuous dispersion and aggregation of oil droplets. It found that HCl molecules only dissociate into solvated H 3 O +… Cl − ion pairs on the surface of concentrated hydrochloric acid, but not H 3 O + and Cl − ions respectively. The concentration of dissociated H 3 O + ions at the interface is lower than that in the bulk phase. The protonation of the A336 molecule promotes the migration of dissociated H 3 O + ions in the bulk phase towards the interface. Because the PdCl 4 2− anions are more likely to be hydrated than PtCl 6 2− anions and combine with H 3 O + ions, the orderly migration of H 3 O + ions in the laminar boundary layer towards the interface drives the mass transfer of easily hydrated PdCl 4 2− anions. The anion exchange between PdCl 4 2− and Cl − ions associated with the A336 molecules results in a higher concentration of Cl − ions enriched at the interface than that in the bulk phase. The migration of easily hydrated Cl − ions towards the bulk phase would drag the water molecules around PtCl 6 2− anions and therefore inhibit the mass transfer of PtCl 6 2− anions. The orderly reverse migration of H 3 O + and Cl − ions enhances the separation between easily hydrated PtCl 6 2− and hardly hydrated PdCl 4 2− anions. This study offers a new perspective on the dissociation of species on the surface of concentrated hydrochloric acid and its impact on separation processes.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Tianrui Xu,Guanghui Wang,Zehua Liu,Nansheng Deng,Xuewen Zhang
A green, efficient and recyclable magnetic BiFeO 3 /Cl-g-C 3 N 4 photocatalyst was prepared for the simultaneous removal of Cr(Ⅵ) and tetracycline (TC) from water by wet chemical and thermal synthesis methods. Experimental results revealed that BiFeO 3 /Cl-g-C 3 N 4 achieved a removal efficiency of 96.1 % for Cr(Ⅵ) and 98.2 % for TC under visible light irradiation for 50 min at pH 6. The results of the work function, charge density difference, UV–vis DRS, PL, PC and EIS tests indicate the formation of S-scheme heterojunctions between BiFeO 3 and Cl-g-C 3 N 4 , which exhibits superior carrier separation and migration efficiency. The evidence for interfacial charge transfer from BiFeO 3 to Cl-g-C 3 N 4 within BiFeO 3 /Cl-g-C 3 N 4 was further corroborated by means of ISIXPS, EPR and KPFM. Moreover, calculations of the density of states demonstrate that the introduction of Cl enhances the reduction capability of BiFeO 3 /Cl-g-C 3 N 4 . Results from ESR tests and trapping experiments has demonstrated that the singlet oxygen ( 1 O 2 ) and electrons are the primary active species. Furthermore, the high removal rates of TC and Cr(VI) from industrial wastewater and groundwater, coupled with the lower ecotoxicity of TC degradation intermediates, indicate that BiFeO 3 /Cl-g-C 3 N 4 has the potential for practical applications. After five cycles, the BiFeO 3 /Cl-g-C 3 N 4 still removed 90.5 % of TC and 96 % of Cr(Ⅵ).
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
·
IF 8.4
Tianrui Xu,Guanghui Wang,Xuewen Zhang,Nansheng Deng
Within the domain of animal husbandry, the misuse of antibiotics in conjunction with elevated levels of heavy metals in feed has led to the contamination of agricultural soils with these metals and antibiotics. In this study, S-scheme heterojunction photocatalyst, BiFeO 3 /Cl-g-C 3 N 4 , was synthesized for the photochemical remediation of tetracycline (TC) and Cr(Ⅵ) in co-contaminated soil, utilizing pyrolysis methods. Following an 8-h photocatalytic reaction, 89.6 % of TC and 75.7 % of Cr(Ⅵ) were effectively removed in soil with the application of BiFeO 3 /Cl-g-C 3 N 4 at a mass ratio of 5 %. The diversity of microbial communities in the remediated soil increased, with a shift in dominant genera from redox bacteria to nutrient bacteria associated with carbon and nitrogen cycling. Moreover, the incorporation of BiFeO 3 /Cl-g-C 3 N 4 in the remediation of soil contamination at depths ranging from 0 to 20 cm resulted in reductions of 40.2 % and 50 % in TC and Cr(Ⅵ) concentrations in subsoil layers, respectively, after 21-days of sunlight irradiation. In comparison to the contaminated group soil, soil from the remediation treatment demonstrated increased growth potential for cabbage and spinach. This work definitely demonstrates that this soil photochemical remediation method based on BiFeO 3 /Cl-g-C 3 N 4 is technologically feasible and has immense potential in the application of remediation of organic pollutants and heavy metals co-contaminated soils.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Shujuan Zhang,Yanpeng Mao,Jian Sun,Tinglu Song,Zhanlong Song,Xiqiang Zhao,Wenlong Wang
In this research, N, Cl doped carbon quantum dots (CQDs) with triple-fluorescence centers was prepared by one-pot solvothermal method from waste traditional Chinese medicines as the raw material. The obtained N, Cl doped CQDs showed purple, yellow and red fluorescence under the 326, 380 and 578 nm excitation, respectively, of which red fluorescence was induced by the increase of concentrations and sensed rapidly water contents in 30–100% range with a limited of detection (LOD) of 0.65%. The obtained CQDs was applied for sensing Cr (Ⅵ) by triple channels, which exhibited the high selectivity and sensitivity for Cr (Ⅵ) with the LOD of 0.28, 0.87 and 0.90 μM, respectively. And its derivative materials exhibited the good linear range with 10–100 μM and 5–250 μM taking purple fluorescence as the response signal, respectively. The recoveries of N, Cl doped CQDs in tap water and sludge were in 93–110% range, suggesting a feasible avenue for accurate and rapid sensing of Cr (Ⅵ).
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Longde Jiang,Jingde Luan,Yu Zhang,Qingyu Chi,Wengang Liu,Zheng Yan,Shaobai Li,Chen Zhao
Phosphorus-oxygen co-doped graphite carbon nitride (POx-CN) are successfully fabricated by in situ impregnation and two-stage thermal polycondensation to investigate the effect of Na + and Cl - on the photocatalytic hydrogen evolution from artificial seawater splitting. The as-prepared POx-CN exhibits a hydrogen evolution rate of 1054.29 μmolg −1 h −1 in artificial seawater , lower than fresh water , indicating that Na + and Cl - play an inhibitory effect on hydrogen evolution reaction . The theoretical calculation indicates that the phosphorus-oxygen binary doping changed the electrostatic potential of the modified layer in carbon nitride molecule, accelerating the electron transfer rate from the structural O in triazine ring to P-N bond. In artificial seawater, the competition between Na + and Pt 2+ at active sites in the modified layer and electron capture by Cl - in the mutual conversion of Cl - and chlorine radicals result in the reduction of hydrogen evolution efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yujie Zhang,Xin He,Haomiao Li,Wenjie Zhao,Kangli Wang,Kai Jiang
Rechargeable magnesium battery is regarded as the promising candidate for the next generation of high-specific-energy storage systems. Nevertheless, issues related to severe Mg-Cl dissociation at the electrolyte–electrode interface impede the insertion of Mg 2+ into most materials, leading to severe polarization and low utilization of Mg-storage electrodes. In this study, a metal–organic polymer (MOP) Ni-TABQ (Ni-coordinated tetramino-benzoquinone) with superior surface catalytic activity is proposed to achieve the high-capacity Mg-MOP battery . The layered Ni-TABQ cathode, featuring a unique 2D π-d linear conjugated structure, effectively reduces the dissociation energy of Mg x Cl y clusters at the Janus interface, thereby facilitating Mg 2+ insertion. Due to the high utilization of active sites, Ni-TABQ achieves high capacities of 410 mAh/g at 200 mA g −1 , attributable to a four-electron redox process involving two redox centers, benzoid carbonyls, and imines . This research highlights the importance of surface electrochemical processes in rechargeable magnesium batteries and paves the way for future development in multivalent metal-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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