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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Selective electrooxidation of 2-hydroxybenzyl alcohol coupled with H2 production promoted by surface reconstruction of β-Ni(OH)2 nanosheets

Weiwei Yang,Mao Peng,Ye Lv,Mengya Sun,Jinli Zhang,Wei Li,Yan Fu

2-Hydroxybenzaldehyde (SALD) exhibits special reactivity in various chemical reactions due to the existence of aldehyde and hydroxyl groups, which also make it a challenge to achieve high conversion and selectivity for SALD production. Herein, β-Ni(OH) 2 nanosheets over nickel foam (NF) at different hydrothermal temperatures were synthesized for electrocatalytic oxidation (ECO) of 2-hydroxybenzyl alcohol (SAL) into SALD. The β-Ni(OH) 2 electrode obtained at 160 °C achieves the best ECO performance in 2.5 M KOH at the applied potential of 1.45 V (RHE), showing the SALD selectivity of 78.90% and the Faradaic efficiency of 87.94% at the SAL conversion of 69.76%. ECO of SAL reduces the cell voltage and boosts the hydrogen productivity by 2.74 times. It is of great importance to find that potential-driven surface reconstruction of β-Ni(OH) 2 enables selective conversion of SAL into SALD. Side reactions including OER as well as oxidation of phenolic group can be effectively controlled via regulating applied potentials on β-Ni(OH) 2 . This work is the first report on direct electrochemical oxidation of SAL with high SALD selectivity, and offers a green and clean strategy for highly selective production of SALD under mild conditions.

CAS / MDL: 12125-01-8 90-01-7
研究领域: 电化学 · 催化 · 材料科学 · 绿色化学
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PROGRESS IN ORGANIC COATINGS · 2024 · IF 6.5

Composite coatings based on silicone-modified polyurethane and marine natural product chlorogentisyl alcohol for marine antifouling

Yuan Feng,Zi-Hao Chen,Yong-Yin Cui,Ming-Yang Zhang,Miao-Qing Sheng,Hui-Jing Li,Yan-Chao Wu

Marine biofouling has a serious impact on marine facilities, and traditional antifoulants may cause secondary pollution to the ocean. As chlorogentisyl alcohol (3-chloro-2,5-dihydroxybenzyl alcohol, CHBA) is a marine natural product with excellent antifouling properties, CHBA and its analogues are prepared and combined with silicone-modified polyurethane (SiPU) for development of potential green composite coatings for marine antifouling. Lubricant polydimethylsiloxane and antifoulant CHBA endow the composite material with antifouling properties under dynamic and static conditions, respectively. CHBA is steadily released from the composite coating at a rate of 28 μg/(cm 2 ·d). As one of the CHBA/SiPU composite coatings, SiPU-3 exhibits inspiring activities against Escherichia coli (Gram-negative bacteria), Staphylococcus aureus (Gram-positive bacteria) and Vibrio fischeri (marine bacteria), with all inhibition rates exceeding 90.0 %. This composite coating has high antiprotein adsorption ability and algal inhibition rate, showing desirable antifouling performance for up to 90 d in seawater. This work will provide new possible considerations in the development of marine antifouling coatings using marine natural antifoulants.

研究领域: 海洋生物学 · 材料科学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Internal electric field drives barrier-free singlet oxygen generation on metal-free carbon for dual environmental-organic synthesis applications

Chuanshun Feng,Shuo Chen,Linjie Guan,Guoen Zhang,Feng Lin,Qicheng Zhang,Xiaobin Fan,Wenchao Peng,Yang Li

A metal-free carbon catalyst co-doped with boron and silicon (2B-BCSi) is designed and synthesized in this work. Its custom-engineered internal electric field achieves the barrier-free and selective generation of singlet oxygen ( 1 O 2 ). Guided by theoretical analysis and density functional theory (DFT) calculations, low‑electronegativity heteroatoms were incorporated into the carbon scaffold to an adjacent electric‑field configuration (B δ+ -C-Si δ+ ). By generating an internal electric field-induced molecular tension and leveraging boron-moderated charge transfer, the system circumvents the adsorption constraints of terminal oxygen that limits traditional approaches. Thereby, it facilitates 1 O 2 production from PMS via a novel barrier-free pathway, resulting in unprecedented selectivity for 1 O 2 (>93.6 %). This system demonstrates significant advantages in electron-rich pollutant degradation (0.437 min −1 ) and organic synthesis (242.8 mg h −1 L −1 ), establishing an electric-field engineering paradigm for precise ROS control while providing dual-path solutions for environmental remediation and value-added chemical production.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Axial pyridine coordination-induced Co d-orbital rearrangement boosts peroxymonosulfate activation for singlet oxygen evolution in water remediation

Huan Chen,Yan Zhao,Zhe Zhang,Bo Niu,Yayun Zhang,Donghui Long

In this work, a cobalt phthalocyanine catalyst with axial pyridine coordination anchored on carbon nanotubes (CoPc-Py-CNT) was developed for enhanced peroxymonosulfate (PMS) activation toward singlet oxygen ( 1 O 2 ) evolution. Axial pyridine coordination induces Co 3 d -N 2 p rehybridization, elevating the Co d z 2 orbital energy level to strengthens d-p orbital hybridization with the oxygen atom in PMS, thereby lowering the activation energy barrier for O-O bond cleavage. The CoPc-Py-CNT/PMS system exhibits an 8.3-fold increase in ciprofloxacin degradation rate and nearly quantitative selectivity in aromatic alcohol oxidation to corresponding aldehydes compared to axially unmodified CoPc-CNT. CoPc-Py-CNT maintains excellent performance in both continuous-flow and 50 L pilot-scale water treatment systems, with minimal cobalt leaching (<20 μg L −1 ) and negligible ecotoxicity. This work proposes a tailored symmetry-breaking strategy via axial coordination to modulate the electronic structure of SACs, offering a robust platform for 1 O 2 -mediated water remediation and selective oxidation reactions in green chemistry applications.

研究领域: 环境化学 · 催化 · 材料科学 · 水处理 · 绿色化学 · 配位化学
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PROCESS BIOCHEMISTRY · 2011 · IF 2.648

A glucose-tolerant β-glucosidase from Prunus domestica seeds: Purification and characterization

Lei Chen,Ning Li,Min-Hua Zong

A glucose-tolerant β-glucosidase was purified to homogeneity from prune ( Prunus domestica ) seeds by successive ammonium sulfate precipitation, hydrophobic interaction chromatography and anion-exchange chromatography. The molecular mass of the enzyme was estimated to be 61   kDa by SDS-PAGE and 54   kDa by gel permeation chromatography. The enzyme has a p I of 5.0 by isoelectric focusing and an optimum activity at pH 5.5 and 55   °C. It is stable at temperatures up to 45   °C and in a broad pH range. Its activity was completely inhibited by 5   mM of Ag + and Hg 2+ . The enzyme hydrolyzed both p -nitrophenyl β- d -glucopyranoside with a K m of 3.09   mM and a V max of 122.1   μmol/min   mg and p -nitrophenyl β- d -fucopyranoside with a K m of 1.65   mM and a V max of 217.6   μmol/min   mg, while cellobiose was not a substrate. Glucono-δ-lactone and glucose competitively inhibited the enzyme with K i values of 0.033 and 468   mM, respectively.

CAS / MDL: 90-01-7 138-52-3
研究领域: 植物学 · 生物化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2016 · IF 3.014

Fabrication of continuous ZrB2 nanofibers derived from boron-containing polymeric precursors

XueYu Tao,ShiXiang Zhou,ZhiMei Xiang,Jie Ma,RuiLin Hou,Yabo Zhu,XianYong Wei

Continuous ceramic nanofibers of ZrB 2 were synthesized via electrospinning combining with polymeric precursor method. The electrospinning solution was prepared from the reaction of Polyzirconoxane (PZO) with 2-Hydroxybenzyl alcohol and boric acid followed by the addition of polyvinylpyrrolidone (PVP). The influences of the solution properties and B/Zr molar ratio on electrospinning were investigated. The electrospun precursors and heat-treated nanofibers were characterized by XRD , SEM, EDS , TEM and Raman. The results showed that pyrolysis at 350 °C helped to stabilize the fibers morphology and ZrB 2 nanofibers were obtained by pyrolyzing the precursor fibers at 1400 °C for 2 h in argon. ZrB 2 nanofibers maintained the excellent fibrous morphology in all the samples. ZrB 2 nanofibers are composed of uniformly nanosized ZrB 2 particles. The average crystallite size of ZrB 2 particles using Scherrer equation is 25 nm. The atomic percentages of zirconium and boron in the product formed in argon at 1400 °C were 17.06% and 33.73% respectively, which is very close to the stoichiometric ZrB 2 .

研究领域: 材料科学 · 纳米技术
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FUEL PROCESSING TECHNOLOGY · 2015 · IF 3.352

Distribution coefficient of products from lignin oxidative degradation in organic-water systems

Jingying Pan,Jie Fu,Shuguang Deng,Xiuyang Lu

A study on extraction of 15 kinds of possible lignin degradation products from aqueous solutions was performed by evaluating the distribution coefficients of five different organic-H 2 O systems under different conditions. The experimental results show that the extraction of lignin degradation products from aqueous solutions achieved equilibrium within 30   min; the concentration of the extracted materials and the amount of extractant had a negligible effect on the distribution coefficients. Among the five kinds of extractants investigated in this work, n-butanol was the best solvent for extracting the lignin degradation products, and chloroform had a good selectivity for the extraction of aldehyde. The temperature greatly influenced the distribution coefficients because the distribution coefficients decreased considerably with the extraction temperature. These results provide insights for the degradation of the lignin in a two-phase system.

研究领域: 化学工程 · 生物化学
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ChemCatChem · 2019 ·Vol. 11 ·期 6 ·1779-1788 · IF 4.495

Selective Aerobic Oxidation of Alcohols over Gold-Palladium Alloy Catalysts Using Air at Atmospheric Pressure in Water

Wei Zhang,Ziqiang Xiao,Jiajun Wang,Wenqin Fu,Rong Tan,Donghong Yin

Graphical Alloys of Catalysis ! Synergistic effect in Au−Pd alloy catalysts enhanced selective aerobic oxidation of alcohols using air at atmospheric pressure in water. A series of bimetallic Au−Pd alloy nanoparticles (NPs) with varied Au/Pd molar ratios was supported on Gamma-alumina (γ-Al 2 O 3 ) surface through the co-impregnation-reduction method using HAuCl 4 and PdCl 2 as metal precursors. Characterization results suggested the high dispersion of Au−Pd alloy NPs, as well as the interplay between the two compositions. Benefitting from the synergistic effects of Au−Pd alloying, the bimetallic Au-Pd x @γ-Al 2 O 3 catalysts were highly efficient for selective aerobic oxidation of various alcohols either aromatic or aliphatic in water using air at atmospheric pressure as a sole oxidant without the need for any cocatalyst. Quantitative yields of corresponding aldehydes or ketones were achieved over Au-Pd 1.2 @γ-Al 2 O 3 within 2 h, whereas pure Au@γ-Al 2 O 3 or Pd@γ-Al 2 O 3 was far less efficient. More importantly, the “alloying effect” appeared to stabilize the bimetallic NPs against aggregation and poisoning, which made the Au-Pd x @γ-Al 2 O 3 more stable and reusable in the aerobic oxidation of alcohols.

研究领域: 化学 · 催化材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Phenoxyl mediators improve enzymatic degradation of organic pollutants: Effect and mechanism

Peng Xie,Wang Zhang,Wugao Wu,Zhuanglin Shen,Mingliang Wang,Yuxiao Lai,Yantao Chen,Zhongfan Jia

A mediation strategy can effectively overcome the low reaction activity of enzymes with nonspecific substrates. In this study, we demonstrated how phenol compounds can mitigate the substrate limitation of HRP in catalytic degradation of various organic pollutants. In a classical HRP/H 2 O 2 system, phenol and natural phenolic compounds (4-HBA & pHBA), exhibited up to over 100-fold enhancement in eliminating organic dyes and persistent antibiotics while the loading is only 2–5 wt%. A combination of molecular modelling, docking and frontier orbital energy analysis was employed to elucidate the catalytic performance and mechanism. We revealed that (1) generating phenoxyl radicals required the proximity of mediators to the HRP active centre, and (2) the subsequent efficient radical transfer to pollutants was determined by the large energy gap between the SOMO energy of phenoxyl radicals and the HOMO energy of phenols. When considering phenols as pollutants, we showed a synergistic effect on catalytic degradation of phenols, dyes, and tetracycline with a removal efficiency of 71–92 %. Overall, this work not only demonstrates that phenoxyl mediators can overcome the lower efficiency and substrate-specificity limitations of the HRP/H 2 O 2 system but also revealed their structure-mediation relationship, implying great potential in the biodegradation of diverse pollutants and their mixtures.

研究领域: 环境科学 · 生物化学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-12 · IF 16.6

Highly active, ultra-low loading single-atom iron catalysts for catalytic transfer hydrogenation

An Zhidong,Yang Piaoping,Duan Delong,Li Jiang,Wan Tong,Kong Yue,Caratzoulas Stavros,Xiang Shuting,Liu Jiaxing,Huang Lei,Frenkel Anatoly I.,Jiang Yuan-Ye,Long Ran,Li Zhenxing,Vlachos Dionisios G.

Highly effective and selective noble metal-free catalysts attract significant attention. Here, a single-atom iron catalyst is fabricated by saturated adsorption of trace iron onto zeolitic imidazolate framework-8 (ZIF-8) followed by pyrolysis. Its performance toward catalytic transfer hydrogenation of furfural is comparable to state-of-the-art catalysts and up to four orders higher than other Fe catalysts. Isotopic labeling experiments demonstrate an intermolecular hydride transfer mechanism. First principles simulations, spectroscopic calculations and experiments, and kinetic correlations reveal that the synthesis creates pyrrolic Fe(II)-plN 3 as the active center whose flexibility manifested by being pulled out of the plane, enabled by defects, is crucial for collocating the reagents and allowing the chemistry to proceed. The catalyst catalyzes chemoselectively several substrates and possesses a unique trait whereby the chemistry is hindered for more acidic substrates than the hydrogen donors. This work paves the way toward noble-metal free single-atom catalysts for important chemical reactions.

研究领域: 催化 · 化学工程 · 材料科学 · 物理化学
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