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APPLIED SURFACE SCIENCE · 2025 · IF 6.9

Breaking the linear scaling relation through synergistic modulation of d-band center and spin state via p-d hybridization for enhanced bifunctional oxygen electrocatalysis

Guanhua Zhang,Mingwang Lu,Qitong Sheng,Guangjian Xing,Xiaojing Yang,Xiaofei Yu,Xinghua Zhang,Zunming Lu,Lanlan Li

The development of highly efficient and stable bifunctional electrocatalysts capable of simultaneously catalyzing the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is critical for advancing zinc-air batteries (ZABs). However, the linear scaling relationship (LSR) governing the adsorption energies of oxygen species imposes constraints on the concurrent enhancement of ORR and OER performance. In this study, we report the synthesis of a novel FeSn/NC catalyst that exhibits strong p-d orbital hybridization by incorporating p-block Sn metal into d-block Fe metal. This strategy facilitates the manipulation of the d-band center and enables the effective formation of low-spin (LS) Fe 3+ simultaneously. The regulation of the d-band center is identified as an effective strategy to enhance the adsorption energy of OOH* and OH* intermediates, while the LS Fe 3+ configuration can effectively weaken the adsorption strength of the O* intermediate. Consequently, this p-d hybridized Fe-based catalyst successfully overcomes the constraints imposed by LSR, thereby boosting bifunctional activity for both ORR and OER. The synthesized FeSn/NC catalyst demonstrates exceptional bifunctional performance with a potential difference (ΔE) of 0.65 V between ORR and OER activities. Furthermore, ZAB based on FeSn/NC achieves an impressive peak power density of 186.0 mW cm −2 , while maintaining stable operation over 700 h during cycling tests. This work offers new insights into designing high-performance bifunctional electrocatalysts through strategies involving synergistic modulation of d-band center and spin state.

CAS / MDL: 10025-77-1
研究领域: 电化学 · 材料科学 · 催化 · 能量存储与转换 · 纳米技术
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BIOTECHNOLOGY AND BIOENGINEERING · 2024 · IF 3.5

Development of growth selection system and pocket engineering of d-amino acid oxidase to enhance selective deamination activity toward d-phosphinothricin

Feng Cheng,Ke-Xiang Sun,Xiao-Xiao Gong,Wei Peng,Hua-Yue Zhang,Xi-Hang Liang,Ya-Ping Xue,Yu-Guo Zheng

D-amino acid oxidase (DAAO)-catalyzed selective oxidative deamination is a very promising process for synthesizing l -amino acids including l -phosphinothricin ( l -PPT, a high-efficiency and broad-spectrum herbicide). However, the wild-type DAAO's low activity toward unnatural substrates like d -phosphinothricin ( d -PPT) hampers its application. Herein, a DAAO from Caenorhabditis elegans ( Ce DAAO) was screened and engineered to improve the catalytic potential on d -PPT. First, we designed a novel growth selection system, taking into account the intricate relationship between the growth of Escherichia coli ( E. coli ) and the catalytic mechanism of DAAO. The developed system was used for high-throughput screening of gene libraries, resulting in the discovery of a variant (M6) with significantly increased catalytic activity against d -PPT. The variant displays different catalytic properties on substrates with varying hydrophobicity and hydrophilicity. Analysis using Alphafold2 modeling and molecular dynamic simulations showed that the reason for the enhanced activity was the substrate-binding pocket with enlarged size and suitable charge distribution. Further QM/MM calculations revealed that the crucial factor for enhancing activity lies in reducing the initial energy barrier of the reductive half reaction. Finally, a comprehensive binding-model index to predict the enhanced activity of DAAO toward d -PPT, and an enzymatic deracemization approach was developed, enabling the efficient synthesis of l -PPT with remarkable efficiency.

CAS / MDL: 119-26-6
研究领域: 生物技术 · 酶学 · 蛋白质工程 · 计算生物学 · 化学生物学
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JOURNAL OF CHEMICAL THERMODYNAMICS · 2016 · IF 2.196

Effect of β-alanine and the solvent composition on the solubility of solvate of calcium d-pantothenate containing four molecules of methanol and one molecule of water (D-PC·4MeOH·1H2O)

Dandan Han,Yumin Liu,Xiaona Li,Teng Zhang,Zhenfang Li,Shichao Du,Mingxia Guo,Shijie Xu,Bo Yu,Baohong Hou,Junbo Gong

The solubility of calcium d -pantothenate in (water   +   methanol) mixtures and the effect of β -alanine on the solubility of calcium d -pantothenate in a constant mole ratio of methanol and water was measured from 263.15   K to 303.15   K by the HPLC analysis method ( P   =   0.1   MPa). The solubility of calcium d -pantothenate increased with increasing temperature in all the mixtures at constant composition. Besides, it also increased with mole fraction of water in (water   +   methanol) mixtures at a constant temperature. Additionally, the solubility of calcium d -pantothenate was enhanced by β -alanine at a given temperature. The experimental solubility in (water   +   methanol) mixtures was correlated by the modified Apelblat equation, the ternary NRTL equation and Solubility-Polarity Model. The Apelblat equation, the quaternary NRTL equation and the Cohn equation were adopted to correlate the experimental solubility in the (water   +   methanol   +   β -alanine) mixtures. Worthwhile, the quaternary NRTL equation was first applied to correlating the quaternary solid-liquid equilibrium. It turned out that all the selected models give good performance on solubility prediction.

CAS / MDL: 107-95-9
研究领域: 药物化学 · 物理化学
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ENZYME AND MICROBIAL TECHNOLOGY · 2021 · IF 3.493

Properties of d-allulose 3-epimerase mined from Novibacillus thermophilus and its application to synthesis of d-allulose

Dong-Xu Jia,Chen-Yi Sun,Yi-Ting Jin,Zhi-Qiang Liu,Yu-Guo Zheng,Mian Li,Hong-Yan Wang,De-Shui Chen

Allulose is an epimer of d -fructose with multiple nutritional functions, which can be biologically synthesized from d -fructose employing d -allulose 3-epimerase (DAE). In this study, NCBI database mining approach was applied to screen novel DAEs, and Novibacillus thermophilus DAE (NtDAE) exhibiting a high activity of 273.9 U/(g⋅wet cell weight) was selected for investigation. NtDAE showed optimum reaction temperature and pH at 70 °C and 7.0, respectively. In the presence of Co 2+ , its activity was improved by 100.1 %, and the half-life ( t 1/2 ) values reached up to 846.3, 539.2 and 47.8 min at 40, 50 and 60 °C, respectively. Higher k cat / K m values toward d -allulose indicated that the preferred physiological substrate of NtDAE was d -allulose. The conversion yield of 500 g/L d -fructose to d -allulose at 60 °C achieved 29.7 %, and further enhanced to 51.6 % with adding 1.1 M borate. This study provided a useful guidance of further engineering and application of NtDAE for realization of industrial production of d -allulose.

CAS / MDL: 57-48-7 50-99-7 921-03-9
研究领域: 生物化学 · 食品科学 · 工业微生物学
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BMC MICROBIOLOGY · 2024 ·Vol. 24 ·期 1 ·1-12 · IF 4

Antibacterial activity and mechanisms of D-3263 against Staphylococcus aureus

Liu Xiaoju,Xiong Yanpeng,Peng Renhai,Zhang Yufang,Cai Shuyu,Deng Qiwen,Yu Zhijian,Wen Zewen,Chen Zhong,Hou Tieying

Multi-drug-resistant Staphylococcus aureus infections necessitate novel antibiotic development. D-3263, a transient receptor potential melastatin member 8 (TRPM8) agonist, has potential antineoplastic properties. Here, we reported the antibacterial and antibiofilm activities of D-3263. Minimum inhibitory concentrations (MICs) against S. aureus , Enterococcus faecalis and E. faecium were ≤ 50 µM. D-3263 exhibited bactericidal effects against clinical methicillin-resistant S. aureus (MRSA) and E. faecalis strains at 4× MIC. Subinhibitory D-3263 concentrations effectively inhibited S. aureus and E. faecalis biofilms, with higher concentrations also clearing mature biofilms. Proteomic analysis revealed differential expression of 29 proteins under 1/2 × MIC D-3263, influencing amino acid biosynthesis and carbohydrate metabolism. Additionally, D-3263 enhanced membrane permeability of S. aureus and E. faecalis . Bacterial membrane phospholipids phosphatidylethanolamine (PE), phosphatidylglycerol (PG), and cardiolipin (CL) dose-dependently increased D-3263 MICs. Overall, our data suggested that D-3263 exhibited potent antibacterial and antibiofilm activities against S. aureus by targeting the cell membrane.

CAS / MDL: 57-03-4
研究领域: 微生物学 · 药理学 · 感染病学
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Materials Today Communications · 2019 · IF 1.859

Preparation, mechanical and thermal characteristics of d-Ti3C2/PVA film

Shaogang Liu,Libo Wang,Xiaolong Wang,Lu Liu,Aiguo Zhou,Xinxin Cao

In this study, Ti 3 C 2 was delaminated into 2D single or few monolayers-thick nanomaterials (d-Ti 3 C 2 ) by DMSO intercalation and sonication method. Then, d-Ti 3 C 2 /polyvinyl alcohol (PVA) films were prepared by solution casting process. The structures, thermal stabilities, thermal behaviors, and surface properties of the resulting materials were characterized by X-ray diffractometry (XRD), scanning electron microscopy (SEM), differential scanning calorimetry (DSC), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and Fourier transform infrared spectroscopy (FTIR). Furthermore, the experimental results showed improvements in mechanical and thermal characteristics of d-Ti 3 C 2 /PVA films, as compared to those of pure PVA. The addition of d-Ti 3 C 2 had beneficial effects on the tensile strength , elongation at break, modulus of elasticity , thermal stability, and crystallinity of PVA matrix. With 0.5 wt% of d-Ti 3 C 2 , d-Ti 3 C 2 /PVA composite exhibited the best comprehensive properties.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 纳米技术
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ANALYTICAL BIOCHEMISTRY · 2015 · IF 2.219

Selective recognition of d-tryptophan from d/l-tryptophan mixtures in the presence of Cu(II) by electropolymerized l-lysine film

Fang Wang,Wencheng Gong,Lili Wang,Zilin Chen

Selective recognition of d -tryptophan ( d -Trp) in the presence of Cu(II) was investigated at poly- l -lysine (p-l-Lys) film using electrochemical impedance spectroscopy (EIS) and differential pulse voltammetry (DPV). p-l-Lys film was immobilized on a glassy carbon electrode (GCE) by cyclic voltammetry between 0.0 and 1.9 V in 20 mM phosphate buffer solution (pH 8.6). After the p-l-Lys/GCE electrode was incubated with d -Trp solution containing Cu(II) ions, obvious enhancement of electron transfer resistance and decrease of voltammetric current could be observed. If d -Trp was replaced by l -tryptophan (l-Trp), there was no apparent resistance and current changes. Moreover, no resistance and current changes could be found in the absence of Cu(II). It may be due to the formation of Cu complex with l -lysine and d -tryptophan. Finally, this method was successfully applied to monitoring enantiomeric composition of the d -Trp and l-Trp mixtures.

CAS / MDL: 73-22-3
研究领域: 生物化学 · 分析化学
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LWT-FOOD SCIENCE AND TECHNOLOGY · 2021 · IF 4.952

Enzymatic lipophilization of d-borneol extracted from Cinnamomum camphora chvar. Borneol seed

Zhe Dong,Yu Zhao,Jinliang Chen,Ming Chang,Xiaosan Wang,Qingzhe Jin,Xingguo Wang

Borneol esters have attracted increasing interest due to their potential application in the food industry. In this study, the extraction of d -borneol from Cinnamomum camphora chvar. borneol seed was carried out via steam distillation to gain highly purified d -borneol (99.66%). The lipase-catalyzed lipophilization of extracted d -borneol with oleic acid was performed in a solvent-free system. The influences of lipase type, substrate molar ratio, lipase loading, reaction temperature and reaction time on d -bornyl oleate yield were evaluated. Among four kinds of commercial lipases screened for their esterification efficiency, CRL (lipase from Candida rugose ) displayed the highest catalytic activity in the synthesis of d -bornyl oleate. The yield of more than 95% was obtained under the optimal conditions: substrate molar ratio 1:2 ( d -borneol/oleic acid), lipase loading 8%, reaction temperature 45 °C, reaction time 48 h. The structural identification of d -borneol and product d -bornyl oleate was performed by gas chromatography mass spectrometry (GC-MS) and proton nuclear magnetic resonance spectroscopy ( 1 H NMR). The results showed that the product was confirmed to be d -bornyl oleate and the purity of which was 97.51%. This study will pave the way for d -borneol and its esters application in food industry.

CAS / MDL: 112-80-1
研究领域: 食品科学 · 生物化学
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GREEN CHEMISTRY · 2020 ·Vol. 23 ·期 3 ·1382-1388 · IF 9.48

Regulating TiO2/MXenes catalysts to promote photocatalytic performance of highly selective oxidation of D-xylose

Liang Chen,Yiming Huang,Ren Zou,Jiliang Ma,Yunyi Yang,Tingzhen Li,Mingsai Li,Qi Hao,Haibo Xie,Xinwen Peng

Synthesis of D-xylonic acid, a high value chemical feedstock, from biomass chemicals through a photocatalytic process is of great significance in respect of economical and sustainable concerns, and therefore has aroused considerable attention. Herein, a TiO2/Ti3C2(TT) photocatalyst was designed for the oxidation of xylose to D-xylonic acid under ambient conditions. The photocatalyst is fabricated by in situ growth of TiO2 nano-particles on Ti3C2 nanosheets and exhibits 64.2% of D-xylonic acid yield with excellent stability. The mechanistic study indicates that the electron transfer from TiO2 to Ti3C2 significantly increases the life time of light-induced charge carriers, and hence improved photocatalytic performance.

CAS / MDL: 13463-67-7 7789-24-4
研究领域: 材料科学 · 化学工程 · 可持续化学 · 光催化
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RSC Advances · 2015 ·Vol. 5 ·期 48 ·38783-38791 · IF 3.84

One-step method to produce methyl-D-glucoside from lignocellulosic biomass

Junfeng Feng,Jianchun Jiang,Junming Xu,Zhongzhi Yang

One-pot acid-catalyzed methanolysis was applied to the liquefaction of biomass to obtain a high molar yield of methyl-D-glucoside at moderate temperature in a short time. A high bamboo conversion ratio (85 wt%) of bamboo and high molar yield of methyl-D-glucoside (40.6 mol%) were achieved. The conditions for high yield were methanol/bamboo mass ratio of 7 (350 mL methanol and 40 g bamboo), 2.0 wt% of catalyst, reaction temperature of 200 °C and reaction time of 10 min. Both hemicelluloses and cellulose (holocellulose) in the lignocellulosic biomass can convert into methyl-D-glucoside, a key and stable product. Methanolysis of biomass proved more efficient than its hydrolysis with an acid catalyst under similar reaction conditions, in water glucose yields were reduced to only 2–8 mol%.

CAS / MDL: 624-45-3 1917-64-2
研究领域: 生物化学 · 可再生资源工程
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JOURNAL OF MOLECULAR LIQUIDS · 2013 · IF 1.684

Measurement and correlation of solubility of d-sorbitol in different solvents

Wenbiao Zhi,Yonghong Hu,Wenge Yang,Yumei Kai,Zheng Cao

The solubility of d -sorbitol was measured in methanol, ethanol, n-propanol, n-butanol, THF, acetone, ethyl acetate and acetonitrile at temperatures ranging from 278.15 to 333.15   K under atmospheric pressure by gravimetric method. The solubility data were correlated with modified Apelblat equation and λh equation which showed that the solubility of d -sorbitol in these organic solvents increased with increasing temperature. The thermodynamic properties of the dissolution process, including enthalpy, entropy and Gibbs energy , were calculated by means of van't Hoff analysis and Gibbs equation. According to the experimental results, ethanol showed to be a relatively better solvent in crystallization process of d -sorbitol.

CAS / MDL: 50-70-4
研究领域: 物理化学 · 化工
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Manipulating d-Band Center and d–p Orbital Coupling to Mitigate Adsorption–Desorption Trade-Off for Efficient CO2-to-CO Photoreduction over MOF Nanofibers

Yong Yang,Jianfeng Jiang,Ya-Nan Feng,Zanyong Zhuang,Fei-Fei Chen,Dantong Zhang,Yan Yu

The strong CO 2 adsorption and facile CO desorption are a trade-off issue for CO 2 -to-CO photoreduction pathways. Synchronous optimization of these two steps remains a substantial hurdle and has been less explored. Herein, an O/N mixed coordinated Co-NTA (NTA: nitrilotriacetic acid), featuring an ultralong nanofiber architecture, is reported for efficient CO 2 photoreduction. The mixed coordination can regulate the positions of d -band center of Co sites and also d – p orbital coupling with coordination atoms, which are recognized as main activity descriptors. Consequently, free energies of both steps of CO 2 →*CO 2 and *CO→CO are well optimized, making the CO 2 -to-CO photoreduction pathways more favorable thermodynamically. By contrast, the classic N-coordinated Co-MeIm (MeIm: 2-methylimidazole) and O-coordinated Co-BDC (BDC: 1,4-benzenedicarboxylic acid) suffer from unfavorable CO 2 adsorption and intractable CO desorption, respectively. In addition, achiral NTA molecules can direct the growth of Co-NTA into one-dimensional (1D) nanofibers, while Co-BDC and Co-MeIm possess typical 2D nanosheet and 3D polyhedron architectures. The fast electron transport along the axis directions makes charge-transfer kinetics most efficient over 1D Co-NTA. The thermodynamic and kinetic benefits jointly contribute to the 1.8-fold increase in CO production over 1D Co-NTA.

研究领域: 材料科学 · 化学工程 · 环境科学
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