BIOORGANIC CHEMISTRY
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2026
·
IF 4.7
Jinnian Wang,Haoming Zhao,Shijun Tong,Xingjian Zhang,Shuyu Ding,Han Zhang,Zhong-Hua Yang
The industrial production of pyridoxal 5′-phosphate (PLP)—an indispensable enzymatic cofactor—is hampered by inefficient multistep chemical syntheses and the economic infeasibility of ATP-dependent biocatalytic routes. To address these challenges, we report an ATP-autonomous biocatalytic cascade that couples pyridoxal kinase (PLK) with polyphosphate kinase (PPK) for sustainable PLP synthesis. This system harnesses inexpensive sodium hexametaphosphate (SHMP) as a phosphoryl donor to drive continuous ATP regeneration, thereby enabling efficient phosphorylation of pyridoxal to PLP without exogenous ATP input. Recombinant PLK and PPK were co-expressed in E. coli BL21(DE3), yielding specific activities of 50 and 145 U/g cell , respectively. The whole-cell biocatalyst achieved only about 25% conversion yield due to mass transfer limitations and intracellular PLP degradation. Notably, while the optimized cell-free system (45 °C, pH 6.5, PLK:PPK = 1:3, 25 mM SHMP) attained a remarkable 95% PLP yield. This 3.8-fold enhancement demonstrates the critical advantage of eliminating cellular barriers in complex multi-enzyme cascades. Our work establishes a robust, ATP-independent platform for high-efficiency PLP biosynthesis that seamlessly integrates cofactor regeneration with cascade catalysis, offering a scalable and economically viable route for industrial biomanufacturing. Moreover, it demonstrates the broader utility of polyphosphate-driven energy recycling in sustainable biocatalysis.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2026
·
IF 3
Sheng Zhizheng,Zhou Jian,Ye Zhaoqi,Wang Tingting,Wang Weihua,Wang Yangdong,Teng Jiawei,Xie Zaiku
Mass transfer on surface of nano-zeolites plays an important impact on their catalytic performance. In this work, we investigated a diffusion-controlled strategy to regulate the interface effect and the dynamic behavior of guest molecules at the interface of nanoZSM-5 via chemical deposition of different silicon (Si) or tungsten (W) species, thereby affecting its performance in methanol to propylene (MTP) reaction. It was verified that only about 1% of sedimentary species form stable surface structures by binding with surface hydroxyl groups and defect hydroxyl groups. Under a pressure of 0.2–5 kPa, Si and W modification respectively increased the surface diffusion efficiency of methanol by 50% and decreased it by 60%, demonstrating the bidirectionality of the control strategy. Meanwhile, acidity and structural characterization confirmed that these properties were not strongly affected. Catalytic results showed that surface diffusion enhancement increased the selectivity of ethylene and propylene, and remained stable within 120 h. Mechanism studies have shown that the dynamics of the accumulated surface species is a key intermediate process that connects surface diffusion and catalytic performance.
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PHOSPHORUS SULFUR AND SILICON AND THE RELATED ELEMENTS
·
2020
·
IF 1.046
Daoke Yu,Wenbin Chen,Shichao Zhang,Rakesh Chilivery,Fuhai Li,Xupeng Lu,Yibing Song,Yiwen Fang
The synthesis conditions of HZSM-5 zeolite, including crystallization temperature, crystallization time and raw material ratio, were investigated by L32 (48) orthogonal test to specifically optimize its performance in dimethyl ether (DME) aromatization for the first time. Based on the total yield of aromatic products, the synthesis conditions of HZSM-5 zeolite with the best DME aromatization properties were obtained by comprehensive analysis and validation experiments. The relationship between the aromatization performance, crystalline structure, pore structure, and acidity of HZSM-5 zeolite were analyzed. The results showed that the HZSM-5 zeolite accompanied by hierarchical structure, an appropriate Brønsted and Lewis acid content and uniform crystal morphology, was successfully synthesized under optimized conditions. Over this unmodified and un-doped catalyst, the conversion of DME approached to 99.3% and the total yield of aromatics reached was 53.5%.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Xiangyang Yuan,Yinmin Cai,Lixi Chen,Shihang Lu,Xin Xiao,Lihua Yuan,Wen Feng
As pre-organized multidentate extractants, phosphine oxides functionalized pillar[5]arenes (POP5As) have showed superior efficiency for uranyl extraction. In this work, the effect of type of organic diluents including dichloromethane (DCM), 1,2-dichloroethane (DCE), 1-nitro-3-(trifluoromethyl)benzene (NTFB) and nitropropane (NP) with different polarity and the fundamental thermodynamic behaviour were investigated in the solvent extraction of uranyl by POP5As from nitric acid (1 M) solution. The extraction ability pertaining to spacer length ( C n H 2n , n = 2, 4, 6), diluent polarity and temperature has been evaluated by comparing the distribution coefficients. The extractant with longer spacer exhibited a better performance in all diluents examined. Particularly, influencing factors including structural variation of ligands and property of organic diluents for the extraction efficiency were discussed from the thermodynamic point of view (Δ H , Δ S and Δ G ). Generally, the extraction processes of uranyl by POP5As were exothermic and spontaneous in nature. In the case of DCE , NTFB and NP, Δ H < 0 and Δ S < 0, the extraction process of uranyl is enthalpy driven whereas the entropy factor counteracts it. In DCM , Δ H < 0 and Δ S > 0, the extraction is synergistically driven by enthalpy and entropy.
研究领域:
超分子化学
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核化学
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溶剂萃取
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热力学
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环境修复
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ACS Catalysis
·
2025
·
IF 13.1
Xu Li,Guodong Qi,Richard J. Lewis,Mark J. Howard,Barry A. Murrer,Brian Harrison,David J. Morgan,Christopher J. Kiely,Qian He,Thomas E. Davies,David J. Willock,Michael Bowker,Jingxian Cao,Feng Deng,Jun Xu,Graham J. Hutchings
The selective oxidation of methane to form methanol and acetic acid has been studied using AuPd nanoparticles supported on the zeolite H-ZSM-5 in water at 240 °C using molecular oxygen as the terminal oxidant in the absence of any added coreductant. The addition of Pd to Au/ZSM-5 significantly increases the selectivity to acetic acid to levels approaching almost complete selectivity within the oxygenated products. However, we observe that the reaction conditions employed lead to the corrosion of the stainless-steel components of the autoclave reactor and also leaching of iron from the ZSM-5 zeolite, and hence the AuPd nanoparticles, on reaction, become coated or partially coated with an oxidic Fe shell. The presence of the oxidized iron coating hinders nanoparticle agglomeration preventing deactivation of the AuPd/ZSM-5 catalyst but does not adversely affect the observed catalysis.
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Small
·
2013
·Vol. 9
·期 19
·3224-3229
·
IF 7.823
Yu-Long Sun,Ying-Wei Yang,Dai-Xiong Chen,Guan Wang,Yue Zhou,Chun-Yu Wang,J. Fraser Stoddart
Graphical Mechanized silica nanoparticles, equipped with pillar[5]arene-[2]pseudorotaxane nanovalves , operate in biological media to trap cargos within their nanopores, but release them when the pH is lowered or a competitive binding agent is added. Although cargo size plays an important role in cargo loading, cargo charge-type does not appear to have any significant influence on the amount of cargo loading or its release. These findings open up the possibility of using pillar[n]arene and its derivatives for the formation of robust and dynamic nanosystems that are capable of performing useful functions.
研究领域:
纳米技术
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材料科学
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生物医学工程
·
化学
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JOURNAL OF ELECTRONIC MATERIALS
·
2019
·Vol. 48
·期 11
·7068-7075
·
IF 1.676
Li Shuhui,Zhou Ying,Cui Lijun,Ge Zhenhua,Feng Jing
In 2 O 3 (ZnO) k superlattice ceramics are promising oxide thermoelectric materials, as superlattice interfaces are effective in scattering phonons and filtering low-energy electrons to decrease thermal conductivity and improve the figure of merit ( ZT ) value. In this work, homologous compounds were prepared by solid-state reaction method using ZnO and In 2 O 3 as raw materials. Phase purity and crystal structure were characterized by x-ray diffraction, revealing that In 2 O 3 (ZnO) k crystallizes in an R3 m space group for odd k values and P6 3 /mmc for even k values. The study of thermoelectric (TE) properties showed that as k increased, the thickness of InO(ZnO)
+ 3
also increased, while the electrical conductivity, thermal conductivity, Seebeck coefficient, power factor and ZT value were all decreased. In 2 O 3 (ZnO) 3 samples obtained a maximum power factor of 651 μ W m −1 K −2 at 973 K, and also achieved a maximum ZT value of 0.24 at 973 K.
研究领域:
材料科学
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凝聚态物理
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能源转换技术
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SCRIPTA MATERIALIA
·
2013
·Vol. 69
·期 8
·574-577
·
IF 2.821
Limeng Liu,Lianbing Zhong,Baoyou Zhang,Zhonghong Lai,Feng Ye,Zhiguo Zhang,Yu Zhou
The effects of the addition of 5 mol.% aluminum , copper, silver or gold on the densification , microstructures, mechanical properties and oxidation resistance in thin air of TaC ceramics were investigated. Full density and relatively high flexural strength (up to 738 MPa) were observed in the case of the Au addition after spark plasma sintering at 1700 °C for 5 min under 30 MPa pressure. Due to wetting of the TaC grains by a thin metallic film , the consolidated materials showed enhanced oxidation resistance against thin air.
研究领域:
材料科学
·
陶瓷
·
冶金学
·
高温材料
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhang Yakun,Xu Lin,Wang Wen,Wu Qing,Zhang Yi
The efficient conversion of ethane has attracted more and more attention because of the shale gas revolution. The coupling of ethane dehydrogenation (EDH) and benzene alkylation over the 1.5Pt/HZSM-5 realize high activity close to the thermodynamic equilibrium of EDH at 500 ℃ and 0.9 bar ethane partial pressure. Meanwhile, the coupled reaction shows long-term stability during 22 h with a slightly decreased ethane conversion of 0.03% per hour and as high as 42% selectivity of ethylbenzene. Based on various characterization, including XRD, HR-TEM, NH 3 -TPD, Py-IR, TGA, it is confirmed that the coupling reaction could convert ethylene, formed by EDH over Pt sites, to ethylbenzene via benzene alkylation over Brönsted acidic sites (BAS) subsequently, and suppressing the sintering of Pt species and coke deposition induced by aromatization and deep dehydrogenation, resulting in high activity and long-time steady state. Graphical Abstract
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Xiao Liu,Yuan Zhang,Peng Zhang,Kang Ge,Ruzhi Zhang,Yixin Sun,Yang Sheng,Mark Bradley,Rong Zhang
Photodynamic therapy (PDT) using 5-aminolevulinic acid (5-ALA) is an important approach for the treatment of some skin diseases and cancers. A major defect of this approach is that it is difficult for 5-ALA to accumulate around lesions in deeper regions of tissue, resulting in poor conversion to the active fluorophore and photodynamic efficiencies. Because of their targeting and controlled release abilities, nanogel carriers could solve this problem. In this paper, nanogels were prepared by using micro-emulsion polymerization with various biodegradable polyester crosslinkers ( L -lactide and ε-caprolactone). The swelling and degradation properties and entrapment efficiency, drug loading and drug release ability of the nanogels were investigated. Nanogels co-cultured with skin cancer cells (A2058) allowed the efficiency of the PDT in vitro to be demonstrated. The results showed that the swelling rate of hydrogels reduced with increasing crosslinker levels, which caused a slow-down in the release of 5-ALA, but lipase accelerated degradation of nanogels increased 5-ALA concentrations in tumor cells and leading to higher PDT efficiency. It was proved by in vivo experiment indicating that the development of skin cancer tissues were efficiently inhibited by the 5-ALA loaded nanogels.
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Chemical Engineering and Processing-Process Intensification
·
2023
·
IF 4.3
Xi-shuo Wang,Ying-jiao Li,Ting-ting Qi,Ji-wen Fu,Guang-Wen Chu,Bao-chang Sun
In industry, H-type zeolites are usually synthesized under hydrothermal conditions in the sodium-containing system, in which great deal of ammonia nitrogen wastewater will be produced during the transformation of zeolites from Na-type to H-type. In this work, we prepared ZSM-5 zeolites in the sodium-free system using organic amines in a rotating packed bed (RPB), which can greatly reduce the amount of wastewater. It was found that the ZSM-5 zeolites synthesized by isopropanolamine (MIPA) had the highest acid amount with a value of 2.331 mmol/g compared to that by other three amines, and exhibits the highest conversion of benzaldehyde with a value of 77.63% in the acetal reaction of benzaldehyde and ethylene glycol . More importantly, RPB premixing can improve the transfer of Al into the framework of ZSM-5 zeolites relative to conventional stirring technique. This work provided a new route to prepare ZSM-5 zeolites with high acid amount in sodium-free system.
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Wu Jinsheng,Yang Ruinan,Zhao Shiqiang,Chen Wei,Chen Zhiyong,Chang Chun,Wu Haoran
The development of mild strategies to transform of fructose to prepare high-purity 5-hydroxymethylfurfural (HMF) is of great significance for biomass valorization, and the design of an efficient catalytic approach is crucial. Herein, a mild catalytic strategy was developed to achieve the preparation of high-purity HMF from fructose over Amberlyst-15 catalyst in a water-methyl isobutyl ketone (MIBK) biphasic system under atmospheric pressure and lower temperature (90 °C). The catalytic system was optimized and analyzed by response surface methodology and kinetics study. Results indicated that a 46.6% yield of HMF could be obtained under optimal conditions: 80 wt% Amberlyst-15 catalyst, the mass ratio of MIBK to H 2 O 10, and the reaction time of 7 h. Furthermore, a simple and efficient purification strategy of HMF was established. High purity (99.0%) and recovery rate (65.5%) of HMF were obtained. This work provides an efficient catalytic strategy to produce high-purity HMF from fructose under atmospheric pressure and lower temperature.
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