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Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo Wu Ximing Yan yuhe liao Hu Li National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion Heterogeneous catalysis Lignin Dual-atom catalyst Selective C-ocleavage

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Engineering versatile Au-based catalysts for solar-to-fuel conversion

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能源化学:英文版 2023年第8期83卷 341-362,I0010页

作者： Chunhua Wang Hongwen Zhang Feili Lai Zhirun Xie Yun Hau Ng Bo Weng Xuejiao Wu yuhe liao Department of Chemistry KU LeuvenCelestijinenlaan 200F3001 LeuvenBelgium cMACS Department of Microbial and Molecular SystemsKU LeuvenCelestijnenlaan 200F3001 LeuvenBelgium School of Energy and Environment City University of Hong Kong83 Tat Chee AvenueKowloonHong Kong 999077China Centre for Sustainable Catalysis and Engineering Faculty of Bioscience EngineeringKU Leuven3001 LeuvenBelgium Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Gold(Au) nanostructures(NSs) have been widely employed as cocatalysts to improve the photoactivity of semiconductor materials, while a systematic summary of the engineering approaches of Au NSs to maximize the solar-to-fuel conversion efficiency is still lacking. In this review, the recently developed strategies for elevating the overall photocatalytic performance of Au-based catalysts and the deep physical chemistry mechanisms are highlighted. Firstly, the synthetic approaches of Au NSs are summarized, followed by an elaboration on their multiple functions in improving photoactivity. Afterward, modification strategies of Au NSs used to enhance the photocatalytic efficiency of Au-semiconductor composites,including controlling the Au NSs morphology, size, crystal phase, defect engineering, alloying with different metals, modulating interfacial interaction, and introducing an external field, are summarized and discussed independently. Additionally, advanced characterization techniques that can provide insights into the charge dynamics of the photocatalysts are introduced. Finally, we share our opinion on the challenges and outline potentially promising opportunities and directions for efficient Au-based photocatalysis research moving forward. We sincerely look forward to this review can deliver insightful views to design efficient Au-based photocatalysts and spur certain innovations to other metal-based catalysts.

关键词： Au nanostructures Modification strategies Semiconductor Photocatalysis Solar-to-fuel conversion

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Fabrication of a sinter-resistant Fe-MFI zeolite dragonfruit-like catalyst for syngas to aromatics conversion

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Journal of Energy Chemistry 2023年第2期77卷 70-79,I0003页

作者： Chenguang Wang Chengyan Wen Zheng Liang Zhipeng Tian Qian Jiang yuhe liao Xunzhu Jiang Lungang Chen Qiying Liu Longlong Ma Michiel Dusselier Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina Southeast University School of Energy and EnvironmentNanjing 210009JiangsuChina Center for Sustainable Catalysis and Engineering(CSCE) KU LeuvenCelestijnenlaan 200F3001 HeverleeBelgium CAS Key Laboratory of Renewable Energy Guangzhou 510640GuangdongChina Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development Guangzhou 510640GuangdongChina University of Chinese Academy of Sciences Beijing 100049China

Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.

关键词： Syngas Aromatics Sinter resistant Oxide-zeolite catalyst

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Grinding Burn Detection Based on Cross Wavelet and Wavelet Coherence Analysis by Acoustic Emission Signal

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Chinese Journal of Mechanical Engineering 2019年第4期32卷 94-103页

作者： Zheyu Gao Jing Lin Xiufeng Wang yuhe liao Shaanxi Key Laboratory of Mechanical Product Quality Assurance and Diagnostics Xi'an Jiaotong University Xi'an 710049China School of Reliability and Systems Engineering Beihang University Beijing 100191 China

Grinding burn monitoring is of great importance to guarantee the surface integrity of the workpiece. Existing methods monitor overall signal variation. However, the signals produced by metal burn are always weak. Therefore, the detection rate of grinding burn still needs to be improved. The paper presents a novel grinding burn detection method basing on acoustic emission(AE) signals. It is achieved by establishing the coherence relationship of pure metal burn and grinding burn signals. Firstly, laser and grinding experiments were carried out to produce pure metal burn signals and grinding burn signals. No-burn and burn surfaces were generated and AE signals were captured separately. Then, the cross wavelet transform(XWT) and wavelet coherence(WTC) were applied to reveal the coherence relationship of the pure metal burn signal and grinding burn signal. The methods can reduce unwanted AE sources and background noise. Novel parameters based on XWT and WTC are proposed to quantify the degree of coherence and monitor the grinding burn. The grinding burn signals were recognized successfully by the proposed indexes under same grinding condition.

关键词： Grinding burn Cross wavelet transform Wavelet coherence Acoustic emission

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结合多种子区域生长和边界延伸的智能牙齿分割方法研究

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生物医学工程学杂志 2024年第3期41卷 520-526页

作者：刘志华薛久涛唐浩廖与禾西安交通大学现代设计及转子轴承系统教育部重点实验室西安710049 西安交通大学陕西省机械产品质量保障与诊断重点实验室西安710049 重庆科技大学机械与动力工程学院重庆401331

三维牙颌模型的分割是计算机口腔辅助诊疗系统的关键步骤。针对牙齿分割技术普适性差、欠分割的问题,提出一种结合多种子区域生长和边界延伸的智能牙齿分割方法。该方法结合牙齿的负曲率网格的分布特点获得新种子点,通过差异性区域生长... 详细信息

三维牙颌模型的分割是计算机口腔辅助诊疗系统的关键步骤。针对牙齿分割技术普适性差、欠分割的问题,提出一种结合多种子区域生长和边界延伸的智能牙齿分割方法。该方法结合牙齿的负曲率网格的分布特点获得新种子点,通过差异性区域生长适应了牙齿顶面和侧面间的差异性结构,并结合几何特征对初次分割的边界进行延伸,有效弥补了区域生长的欠分割缺陷。在实验中,通过与当前经典的算法进行对比和消融实验,表明本文方法能够更好地分割拥挤的牙颌模型,具有较强算法普适性,已具备满足口腔诊疗中实际分割需求的能力。

关键词：牙齿分割区域生长算法多种子点边界延伸

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碳纳米管修饰气体扩散电极高效电化学还原CO_(2)

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工程热物理学报 2024年第2期45卷 494-499页

作者：钟立阳邓雨荷付乾李俊张亮朱恂廖强重庆大学低品位能源利用及系统教育部重点实验室重庆400030 重庆大学工程热物理研究所重庆400030

电化学还原CO_(2)可利用可再生能源实现CO_(2)转化,是实现碳中和目标的重要支撑,但目前其反应器存在法拉第效率较低和槽电压较高等问题,严重制约其发展。本文用碳纳米管修饰催化层从而构建了新型气体扩散电极,研究发现添加碳纳米管后电... 详细信息

电化学还原CO_(2)可利用可再生能源实现CO_(2)转化,是实现碳中和目标的重要支撑,但目前其反应器存在法拉第效率较低和槽电压较高等问题,严重制约其发展。本文用碳纳米管修饰催化层从而构建了新型气体扩散电极,研究发现添加碳纳米管后电极在200 mA·cm^(-2)的电流密度下CO法拉第效率最高可达93%,槽电压仅为-2.42 V,相较未添加碳纳米管的电极法拉第效率提高了13.7%,槽电压降低了240 m V,传荷阻力减小了29.4%。其主要原因是碳纳米管交错所形成的疏水三维骨架网络不仅有利于催化剂颗粒的分散,还有利于催化层孔隙率的提升和CO_(2)传输的增强。

关键词：电化学还原CO_(2) 气体扩散电极流动式反应器碳纳米管

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Sustainable production of value-added N-heterocycles from biomass-derived carbohydrates via spontaneous self-engineering

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National Science Open 2023年第6期2卷 1-16页

作者： Feng Yu Chong Liu Fenghua Tan yuhe liao Liang Wang Yuping Li Feng-Shou Xiao Key Lab of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310028China Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640China

Synthetic N-heterocyclic compounds,such as quinoxalines,have shown a crucial role in pharmaceutical as well as food and dye industries.However,the traditional synthesis toward N-heterocycles relies on multistep energy and costintensive non-sustainable processes.Here,we report a facile approach that allows one-step conversion of biomass-derived carbohydrates to valuable quinoxalines in the presence of aryl-1,2-diamines in water without any harmful metal catalysts/organic solvents via spontaneously engineering involved cascade reactions under hydrothermal conditions.Aryl-1,2-diamines are revealed as the key to propel this transformation through boosting carbohydrate fragmentation into small 1,2-dicarbonyl intermediates and subsequently trapping them for constituting stable quinoxaline scaffolds therefore avoiding a myriad of undesired side reactions.The tunability of product selectivity can be also achievable by adjusting the basicity of the reaction environment.Both batch and continuous-flow integrated processes were verified for production of quinoxalines in an exceptionally eco-benign manner(E-factor<1),showing superior sustainability and economic viability.

关键词： biomass conversion sustainability green chemistry carbohydrate N-heterocycle

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生物质热解动力学模型研究进展

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能源环境保护 2024年第2期38卷 67-80页

作者：李亮朱一萍廖玉河中国科学院广州能源研究所广东广州510640

生物质是地球上最丰富的可再生碳资源之一,在实现“双碳”战略目标方面扮演着重要作用。生物质热解是一项极具前景的生物质利用技术,其中热解形成的生物油有望取代传统化石能源,用于生产高值燃料或化学品。然而,生物质热解是一个十分复... 详细信息

生物质是地球上最丰富的可再生碳资源之一,在实现“双碳”战略目标方面扮演着重要作用。生物质热解是一项极具前景的生物质利用技术,其中热解形成的生物油有望取代传统化石能源,用于生产高值燃料或化学品。然而,生物质热解是一个十分复杂的过程,该过程及热解产物分布受诸多因素影响。因此,发展生物质热解动力学模型对指导热解工艺生产十分重要。动力学模型的研究不仅可以揭示热解过程中所涉及的物理化学变化,还可以预测热解反应速率及主要产物分布。早期构建的全局动力学模型为热解机理的理解与更详细模型的发展奠定了基础。随着生物质热解的主要研究目标由最大化生物油产量转变为最大化高附加值化学品产量,包含更多热解机理信息和可预测更多单个产物产率的半详细和详细动力学模型开始出现。主要介绍了生物质热解动力学模型的研究现状,将动力学模型分为全局模型、半详细模型和详细模型,并对未来生物质热解动力学研究及详细模型的发展进行了展望。

关键词：生物质热解动力学模型高附加值

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左归丸含药血清对Hedgehog-GLi通路关键因子mRNA表达及骨吸收功能的影响

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中国骨质疏松杂志 2024年第6期30卷 807-812页

作者：廖泽绮史婧儒王雨荷赵宏艳张元月刘梅洁中国中医科学院医学实验中心北京100700

目的探讨左归丸含药血清对成骨-破骨细胞共培养体系中Hedgehog-GLi通路关键因子mRNA表达及骨吸收功能的影响。方法建立成骨细胞、破骨细胞、骨磨片共培养体系,实验分为7组:空白对照组、假手术组、OVX组、阳性对照组、左归丸组、激动剂... 详细信息

目的探讨左归丸含药血清对成骨-破骨细胞共培养体系中Hedgehog-GLi通路关键因子mRNA表达及骨吸收功能的影响。方法建立成骨细胞、破骨细胞、骨磨片共培养体系,实验分为7组:空白对照组、假手术组、OVX组、阳性对照组、左归丸组、激动剂组和激动剂+左归丸组。选用50只雌性SD大鼠,分别制备相对应组含药血清,实验各组分别加入相对应组大鼠血清。通过实时荧光定量PCR检测成骨细胞Ihh、Ptch、Smo、GLi1、OPG及RANKL的mRNA表达;并采用甲苯胺蓝染色方法检测破骨细胞骨吸收功能。结果与假手术组相比,OVX组Ihh、Ptch、Smo、GLi1mRNA表达显著上调,同时OPGmRNA表达水平显著降低,RANKL mRNA表达水平显著增加,RANKL/OPG比值明显增高。与OVX组相比,阳性对照组与左归丸组Ihh、Ptch、Smo、GLi1mRNA表达明显下调,同时OPG mRNA表达水平显著升高,RANKL mRNA表达水平显著降低,RANKL/OPG比值明显下降。OVX组加入激动剂Shh重组蛋白后,Hedgehog-GLi信号通路关键因子的mRNA表达较OVX组明显增加。与激动剂组比较,激动剂+左归丸组Ihh、Ptch、Smo、GLi1mRNA表达以及RANKL/OPG比值均明显下降。与假手术组相比,OVX组的骨吸收陷窝面积显著增加;与OVX组相比,阳性对照组和左归丸组的骨吸收陷窝面积显著下降。结论左归丸含药血清可一定程度上抑制Hedgehog-GLi通路关键因子Ihh、Ptch、Smo、GLi1的活性,进而抑制OVX所致的骨吸收增强。

关键词：左归丸骨质疏松症 Hedgehog-GLi信号通路成骨细胞破骨细胞共培养体系

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左归丸含药血清对成骨细胞中Ihh、Ptch、Smo、GLi1蛋白表达及破骨细胞数量的影响

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中国中医基础医学杂志 2024年第6期30卷 998-1004页

作者：史婧儒廖泽绮王雨荷赵宏艳张元月刘梅洁中国中医科学院医学实验中心北京100700

目的探讨左归丸含药血清对成骨细胞中Hedgehog-GLi通路关键蛋白表达及破骨细胞数量的影响。方法选用50只雌性SD大鼠,随机分为空白对照组、假手术组、造模组。造模组大鼠切除双侧卵巢,12周后随机分为卵巢切除组(ovariectomy,OVX)、阳... 详细信息

目的探讨左归丸含药血清对成骨细胞中Hedgehog-GLi通路关键蛋白表达及破骨细胞数量的影响。方法选用50只雌性SD大鼠,随机分为空白对照组、假手术组、造模组。造模组大鼠切除双侧卵巢,12周后随机分为卵巢切除组(ovariectomy,OVX)、阳性对照组和左归丸组。阳性对照组大鼠灌服戊酸雌二醇混悬液,左归丸组大鼠灌服左归丸水煎液,连续干预7 d。末次给药1.5 h后,腹主动脉取血制备各组相应含药血清。建立成骨细胞、破骨细胞、骨磨片共培养体系,分为空白对照血清组、假手术血清组、OVX血清组、阳性对照血清组、左归丸含药血清组、激动剂组和激动剂+左归丸含药血清组,分别添加各组对应血清。免疫荧光法检测成骨细胞印度刺猬蛋白(Indian hedgehog,Ihh)、碎片蛋白(patched,Ptch)、润滑蛋白(smoothened,Smo)及GLi1蛋白表达;免疫组化法检测成骨细胞骨保护蛋白(osteoprotegerin,OPG)、核因子受体激活因子-κB配体(receptor activator for nuclear factor-κB ligand,RANKL)蛋白表达;对破骨细胞进行TRAP染色,计算TRAP+细胞数;ELISA检测共培养体系上清液中TRAP的含量。结果与假手术血清组比较,OVX血清组Ihh、Ptch、Smo、GLi1蛋白表达水平显著上调(P<0.01),RANKL/OPG比值增高;TRAP+细胞数和细胞上清液中TRAP含量亦明显增加(P<0.05)。与OVX血清组比较,左归丸含药血清组Ihh、Ptch、Smo、GLi1的蛋白表达明显下调,RANKL/OPG比值下降;TRAP+细胞数和细胞上清液中TRAP含量明显降低(P<0.05)。与激动剂组比较,加入左归丸含药血清后,Ihh、Ptch、Smo、GLi1的蛋白表达及RANKL/OPG比值均明显下降,TRAP+细胞个数及TRAP含量亦明显降低(P<0.05)。结论左归丸含药血清可通过抑制异常活跃的Hedgehog-GLi信号通路,使Ihh、Ptch、Smo、GLi1的蛋白表达水平下调,降低RANKL/OPG比值,抑制破骨细胞的数量和活性,起到减少骨丢失作用。

关键词：左归丸骨质疏松症 Hedgehog-GLi信号通路成骨细胞破骨细胞

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