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Strain‑Induced Surface Interface Dual Polarization Constructs PML‑Cu/Bi_(12)O_(17)Br_(2) High‑Density Active Sites for CO_(2) Photoreduction

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Nano-Micro Letters 2024年第5期16卷 169-183页

作者： Yi Zhang Fangyu Guo Jun Di Keke Wang Molly Meng‑Jung Li Jiayu Dai yuanbin she Jiexiang Xia Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchSchool of the Environment and Safety EngineeringJiangsu UniversityZhenjiang 212013People’s Republic of China State Key Laboratory Breeding Base of Green Chemistry‑Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014People’s Republic of China College of Science and Hunan Key Laboratory of Extreme Matter and ApplicationsNational University of Defense TechnologyChangsha 410073People’s Republic of China Department of Applied Physics The Hong Kong Polytechnic UniversityHung HomHong KongPeople’s Republic of China School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research CenterNanjing University of Science and TechnologyNanjing 210094People’s Republic of China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Normal UniversityJinhua 321004People’s Republic of China

The insufficient active sites and slow interfacial charge trans-fer of photocatalysts restrict the efficiency of CO_(2) photoreduction.The synchronized modulation of the above key issues is demanding and chal-lenging.Herein,strain-induced strategy is developed to construct the Bi–O-bonded interface in Cu porphyrin-based monoatomic layer(PML-Cu)and Bi_(12)O_(17)Br_(2)(BOB),which triggers the surface interface dual polarization of PML-Cu/BOB(PBOB).In this multi-step polarization,the built-in electric field formed between the interfaces induces the electron transfer from con-duction band(CB)of BOB to CB of PML-Cu and suppresses its reverse migration.Moreover,the surface polarization of PML-Cu further promotes the electron converge in Cu atoms.The introduction of PML-Cu endows a high density of dispersed Cu active sites on the surface of PBOB,significantly promoting the adsorption and activation of CO_(2) and CO desorption.The conversion rate of CO_(2) photoreduction to CO for PBOB can reach 584.3μmol g-1,which is 7.83 times higher than BOB and 20.01 times than PML-Cu.This work offers valuable insights into multi-step polarization regulation and active site design for catalysts.

关键词： Bi_(12)O_(17)Br_(2) Porphyrin CO_(2)photoreduction Polarization Active sites

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基于银纳米三角片蚀刻机制区分不同产地浓香型白酒

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食品工业科技 2024年第10期45卷 254-262页

作者：贾俊杰张宿义许涛马龙黄张君王松涛佘远斌泸州品创科技有限公司/国家固态酿造工程技术研究中心四川泸州646000 泸州老窖股份有限公司四川泸州646000 浙江工业大学化学工程学院浙江杭州310014

区分不同产地白酒对于产品质量控制和原产地保护具有重要意义。本研究以四种不同形貌大小的银纳米三角片(Ag nanoprism,AgNPRs)作为传感材料,两种金属离子和一种氧化阴离子作为氧化蚀刻剂,基于AgNPRs蚀刻机制构建了一种4×3传感阵列,将... 详细信息

区分不同产地白酒对于产品质量控制和原产地保护具有重要意义。本研究以四种不同形貌大小的银纳米三角片(Ag nanoprism,AgNPRs)作为传感材料,两种金属离子和一种氧化阴离子作为氧化蚀刻剂,基于AgNPRs蚀刻机制构建了一种4×3传感阵列,将该阵列对四川、江淮和北方三大产地共41款代表性浓香型白酒样品进行比色响应,所获得的比色信号值通过线性判别分析(linear discriminant analysis,LDA)进行判别分析,并进一步选取了部分未知样品对判别模型进行了外部验证。比色响应机制研究结果表明,白酒样品对AgNPRs的蚀刻效应起促进作用,这可能与白酒中含有不同的有机酸有关。对不同产地样品的区分结果显示,单一阵列对不同产地样品的区分效果相对较低,三种阵列组合后的区分效果明显提高,对41个样品的产地判别率可达99%,对15个未知浓香型酒样的产地判别率可达98%。采用组合阵列对四川产地5种品牌21个样品和江淮产地3种品牌13个样品判别率分别可达99%和100%,采用单一阵列对四川各厂家不同等级产品的判别率均可达100%。本研究采用的纳米比色传感方法简便快速,不仅可用于产品鉴别和防伪,也可辅助用于生产过程质量监控,为白酒质量智能化监控奠定研究基础。

关键词：浓香型白酒银纳米三角片蚀刻机制比色传感阵列模式识别

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Studies on QSAR of metalloporphyrin catalysts in the oxidation of cyclohexane to adipic acid

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Frontiers of Chemical Science and Engineering 2007年第2期1卷 155-161页

作者： CHEN Yixia she yuanbin XU Jing LI Yan Institute of Green Chemistry and Fine Chemicals and Department of Chemistry and Chemical Engineering College of Environmental and Energy EngineeringBeijing University of TechnologyBeijing 100022China

The catalysis of chloridized metalloporphyrins in the oxidation of cyclohexane to adipic acid was systemati-cally investigated.The turnover numbers(TON)data of 19 catalysts were obtained experimentally under optimal reac-tion conditions,and 2.4x106 TON for T(o-Cl)PP-MnIIICl catalyst at 2.0x10–6 mol/L of dosage was reached under the conditions of dioxygen pressure of 2.5 MPa at 150°C for 4 h.This was the best result reported for this reaction up to now.The QSAR models for each concerned metallopor-phyrin were established,where the catalytic activity was significantly correlated with the ELUMO(the energy level of the lowest unoccupied molecule orbit)and LM-N(the bond length between metal-nitrogen atoms).Using the QSAR models,four new metalloporphyrins with substituted nitro group were designed,and their catalytic activities were predicted.The experimental TON data of newly designed porphyrins were in good agreement with the predicted ones,and the square of their correlation coefficient was more than 0.958.The above results demonstrated that the proposed structure-activity relationship model could be applied to design some new metalloporphyrin catalysts,and to predict their catalytic activity in cyclohexane oxidation.

关键词： metalloporphyrin catalyst quantitative structure-activity relationship(QSAR)model cyclohexane oxidation adipic acid

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Electrochemical C-H/N-H cross-coupling of 2-phenylindolizines with phenothiazines to synthesize novel N-aryl phenothiazine derivatives

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Chinese Chemical Letters 2023年第6期34卷 306-309页

作者： Chenglong Feng Xin Liu yuanbin she Zhenlu shen Meichao Li College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310032China

A facile and elegant method for synthesis of novel N-aryl phenothiazine derivatives from 2-phenylindolizines and phenothiazines through direct electrochemical oxidation has been developed.This approach was performed smoothly at room temperature without external oxidant and catalyst.Cyclic voltammetry and in situ FTIR techniques were applied to analyze the cross-coupling process of phenothiazines and 2-phenylindolizines,which helped to select the appropriate reaction potential.Under the optimized conditions,a broad range of substrates were well tolerated,affording the desired products in moderate to excellent isolated yields(up to 91%)with high regioselectivity.Meanwhile,a plausible mechanism involving a radical pathway has been proposed.

关键词： N-Aryl phenothiazine derivatives Electrochemical oxidation 2-Phenylindolizines Phenothiazines Cross-coupling

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A succinct enhanced luminescence strategy for fluorescent ionic liquids and the application for detecting CO_(2)

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Green Energy & Environment 2022年第5期7卷 1093-1101页

作者： Siying Che Jiachen Guo Lu Gan Qiaoxin Xiao Haoran Li yuanbin she Congmin Wang College of Chemical Engineering Zhejiang University of TechnologyHangzhou310014China Department of Chemistry ZJU-NHU United R&D CenterZhejiang UniversityHangzhou310027China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Zhejiang UniversityHangzhou310027China

An interesting phenomenon was found that fluorophore was introduced into ionic liquid(IL)to magnify fluorescence signal via the thermally activated delayed fluorescence process;thus up to 15 fold enhancements were achieved.Hence,we reported a succinct enhanced luminescence strategy to reduce single-triplet energy split by the tunability of ILs.This strategy could be extended to more kinds of ILs by the virtue of a preliminary DFT calculation screening.Moreover,the optical feature of IL sensor made it a promising candidate as a gas fluorescence sensor.

关键词： luminescence ionic liquids

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Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations

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Frontiers of Chemical Science and Engineering 2020年第6期14卷 1052-1064页

作者： Jinhua Zhang yuanbin she College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014China School of Materials and Environmental Engineering Chizhou UniversityChizhou 247000China

In this study,the decomposition of methanol into the CO and H species on the Pd/tungsten carbide(WC)(0001)surface is systematically investigated using periodic density functional theory(DFT)calculations.The possible reaction pathways and intermediates are determined.The results reveal that saturated molecules,i.e.,methanol and formaldehyde,adsorb weakly on the Pd/WC(0001)surface.Both CO and H prefer three-fold sites,with adsorption energies of-1.51 and-2.67 eV,respectively.On the other hand,CH30 stably binds at three-fold and bridge sites,with an adsorption energy of-2.58 eV.However,most of the other intermediates tend to adsorb to the surface with the carbon and oxygen atoms in their sp3 and hydroxyl-like configurations,respectively.Hence,the Catom of CH2OH preferentially attaches to the top sites,CHOH and CH2O adsorb at the bridge sites,while COH and CHO occupy the three-fold sites.The DFT calculations indicate that the rupture of the initial C-H bond promotes the decomposition of CH3OH and CH2OH,whereas in the case of CHOH,O-H bond scission is favored over the C-H bond rupture.Thus,the most probable methanol decomposition pathway on the Pd/WC(0001)surface is CH3OH→ CH2OH→trans-CUOH→CHO→CO.The present study demonstrates that the synergistic effect of WC(as carrier)and Pd(as catalyst)alters the CH3OH decomposition pathway and reduces the noble metal utilization.

关键词： density functional theory methanol direct methanol fuel cells WC(0001)-supported Pd monolayer decomposition mechanism

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Catalyst-free and solvent-free oxidation of cycloalkanes(C5-C8) with molecular oxygen:Determination of autoxidation temperature and product distribution

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Chinese Journal of Chemical Engineering 2018年第5期26卷 1064-1070页

作者： Haimin shen Yan Wang Jinhui Deng Long Zhang yuanbin she State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology College of Chemical Engineering Zhejiang University of Technology

Autoxidation of cycloalkanes(C5–C8) with molecular oxygen under catalyst-free and solvent-free conditions was conducted systematically for the first time, focusing on the autoxidation temperature and product distribution. The autoxidation of cyclopentane, cyclohexane, cycloheptane and cyclooctane occurs at 120 ℃,130 ℃, 120 ℃, and 105 ℃ respectively, with obvious oxidized products formation. At 140 ℃, 145 ℃, 130 ℃ and 125 ℃, acceptable yields of the oxidized products could be obtained for them, and the oxidized product distributions were investigated in detail. The autoxidation of cycloalkanes follows the pseudo-first-order kinetic model and the apparent activation energies(E_a) for the autoxidation of cyclopentane and cyclohexane are 159.76 kJ·mol^(-1) and 86.75 kJ·mol^(-1) respectively. This study can act as an important reference in screen of suitable reaction temperature and comparison of the performance of various catalysts in the catalytic oxidation of cycloalkanes in the attempt to enhance the oxidized product selectivity.

关键词：氧化温度自然氧化产品分布催化剂分子分发溶剂运动模型

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Advances and perspectives in catalysts for liquid-phase oxidation of cyclohexane

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Frontiers of Chemical Science and Engineering 2012年第3期6卷 356-368页

作者： Hui LI yuanbin she Tao WANG Institute of Green Chemistry and Fine Chemicals Beijing University of TechnologyBeijing 100124China

在为环己烷的氧化的催化剂的最近的进步和开发被考察。为包括金属的环己烷的氧化的催化系统支持了，金属氧化物，分子的筛，金属代替的 polyoxometalates，光催化剂， organocatalysts， Gif 系统，金属器官的催化剂和 metalloporphyri... 详细信息

在为环己烷的氧化的催化剂的最近的进步和开发被考察。为包括金属的环己烷的氧化的催化系统支持了，金属氧化物，分子的筛，金属代替的 polyoxometalates，光催化剂， organocatalysts， Gif 系统，金属器官的催化剂和 metalloporphyrins 在 metalloporphyrin 上与一个特别重音被讨论催化系统。这些方法的优点和劣势被总结并且分析。最后，在环己烷的氧化技术的发展趋势被检验。

关键词：氧化环己烷光催化剂金属氧化物有机金属催化剂展望液相多金属氧酸盐氧化反应

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Selective oxidation of o-nitrotoluene to o-nitrobenzaldehyde with metalloporphyrins as biomimetic catalysts

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Frontiers of Chemical Science and Engineering 2009年第4期3卷 453-456页

作者： Xinling WANG yuanbin she Institute of Green Chemistry and Fine Chemicals Beijing University of TechnologyBeijing 100124China

Selective oxidation of o-nitrotoluene to onitrobenzaldehyde with metalloporphyrins as biomimetic catalysts was studied.The peripheral substituent around porphyrin rings and various process parameters of NaOH concentration,reaction temperature,reaction time and oxygen pressure all affect the selectivity of onitrobenzaldehyde.Further,82.0%selectivity of onitrobenzaldehyde was achieved under the optimum conditions:1.0×10^(-5)mol·L^(-1)of T(p-NO_(2))PPFeCl catalyst,2.5 mol·L^(-1)of NaOH,0.2 mol·L^(-1)of o-nitrotoluene,45℃and 2.0 MPa for 6 h.

关键词： o-nitrotoluene o-nitrobenzaldehyde metalloporphyrins

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Selective epoxidation of linear terminal olefins with metalloporphyrins under mild conditions

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Frontiers of Chemical Science and Engineering 2009年第3期3卷 310-313页

作者： Xiaoguang BAI yuanbin she Institute of Green Chemistry and Fine Chemicals Department of Chemistry and Chemical EngineeringCollege of Environmental and Energy EngineeringBeijing University of TechnologyBeijing 100124China

The epoxidation of linear terminal olefins with metalloporphyrins in the presence of dioxygen and isobutyraldehyde under ambient temperature and atmo-spheric pressure was investigated.The results show that all olefins could be smoothly converted to epoxides with high selectivities(70%–90%).For the metalloporphyrins with different catalytic activities within 1-hexene epoxidation in the order of Fe>Mn>Co,T(o-Cl)PPFe(III)Cl was most effective,with a 41.7%yield and 80.2%selectivity of 1,2-epoxyhexane.Various amounts of catalyst were investi-gated,and it was found that with only 10ppm catalyst the yield of 1,2-epoxyhexane and turnover number(TON)could reach up to 41.9%and 41859,respectively.

关键词： metalloporphyrins olefins dioxygen epox-idation

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