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Role of catalyst surface-active sites in the hydrogenation ofα,β-unsaturated aldehyde

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Frontiers of Chemical Science and Engineering 2024年第6期18卷 41-69页

作者： Haixiang Shi Tongming Su Zuzeng Qin hongbing ji School of Chemistry and Chemical Engineering Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification TechnologyGuangxi UniversityNanning 530004China Zhejiang Green Petrochemical and Light Hydrocarbon Transformation Research Institute Zhejiang University of TechnologyHangzhou 310014China

As an important technology in fine chemical production,the selective hydrogenation ofα,β-unsaturated aldehydes has attracted much attention in recent *** the process ofα,β-unsaturated aldehyde hydrogenation,a conjugated system is formed between>C=CC=O,leading to hydrogenation at both ends of the conjugated system,which competes with each other and results in more complex ***,improving the reaction selectivity is also difficult in industrial ***,many researchers have reported that surface-active sites on catalysts play a crucial role inα,β-unsaturated aldehyde *** review attempts to summarize recent advances in understanding the effects of surface-active sites(SASs)over metal catalysts for enhancing the process of *** construction strategies and roles of SASs for hydrogenation catalysts are *** attention has been given to the adsorption configuration and transformation mechanism ofα,β-unsaturated aldehydes on catalysts,which contributes to understanding the relationship between SASs and hydrogenation *** addition,recent advances in metal-supported catalysts for the selective hydrogenation ofα,β-unsaturated aldehydes to understand the role of SASs in hydrogenation are briefly ***,the opportunities and challenges will be highlighted for the future development of the precise construction of SASs.

关键词： α,β-unsaturatedd aldehydes hydrogenation active site cinnamaldehyde

Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu hongbing ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

Systematic engineering of BiVO_(4)photoanode for efficient photoelectrochemical water oxidation

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Carbon Energy 2024年第4期6卷 12-21页

作者： Zhiting Liang Meng Li Kai‐Hang Ye Tongxin Tang Zhan Lin Yuying Zheng Yongchao Huang hongbing ji Shanqing Zhang Guangzhou Key Laboratory of Clean Transportation Energy Chemistry School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhouChina Chemical Engineering Guangdong Laboratory Jieyang Branch of ChemistryJieyangChina Key Laboratory for Water Quality and Conservation of the Pearl River Delta Institute of Environmental Research at Greater Bay AreaMinistry of EducationGuangzhou UniversityGuangzhouChina State Key Laboratory Breeding Base of Green‐Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhouChina School of Environment and Science Centre for Catalysis and Clean EnergyGriffith UniversityGold Coast CampusSouthportQueenslandAustralia

BiVO_(4)is one of the most promising photoanode materials for photoelectrochemical(PEC)solar energy conversion,but it still suffers from poor photocurrent density due to insufficient light‐harvesting efficiency(LHE),weak photogenerated charge separation efficiency(Φ_(Sep)),and low water oxidation efficiency(Φ_(OX)).Herein,we tackle these challenges of the BiVO_(4)photoanodes using systematic engineering,including catalysis engineering,bandgap engineering,and morphology *** particular,we deposit a NiCoO_(x)layer onto the BiVO_(4)photoanode as the oxygen evolution catalyst to enhance theΦ_(OX)of Fe‐g‐C_(3)N_(4)/BiVO_(4)for PEC water oxidation,and incorporate Fe‐doped graphite‐phase C_(3)N_(4)(Fe‐g‐C_(3)N_(4))into the BiVO_(4)photoanode to optimize the bandgap and surface areas to subsequently expand the light absorption range of the photoanode from 530 to 690 nm,increase the LHE andΦ_(Sep),and further improve the oxygen evolution reaction activity of the NiCoO_(x)catalytic ***,the maximum photocurrent density of the as‐prepared NiCoO_(x)/Fe‐g‐C_(3)N_(4)/BiVO_(4)is remarkably boosted from 4.6 to 7.4 mA cm^(−2).This work suggests that the proposed systematic engineering strategy is exceptionally promising for improving LHE,Φ_(Sep),andΦ_(OX)of BiVO_(4)‐based photoanodes,which will substantially benefit the design,preparation,and large‐scale application of next‐generation high‐performance photoanodes.

关键词： bismuth vanadate carbon nitride charge separation heterojunction water oxidation

Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts

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Science China Chemistry 2024年

作者： Ying Zhang Liyang Liu Ziyue Wang Xingcong Zhang Xiaohui He hongbing ji Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of Chemistry IGCME Sun Yat-sen University Guangdong Technology Research Center for Synthesis and Separation of Thermosensitive Chemicals State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon Conversion College of Chemical Engineering Zhejiang University of Technology

Tandem hydroformylation/hydrogenation of olefins to alcohols is an appealing and challenging route that has received continuous interest. Herein, we report a bifunctional atomically dispersed Rh and Co catalyst（RhCo/Al2O3-10） prepared by a simple ball milling method that displays superior synergistic catalytic performance（>95% olefins conversion and >80% alcohols selectivity） and broad substrate scope for tandem hydroformylation/hydrogenation reaction, outperforming Rh/Al2O3, Co/Al2O3,and their physically mixed counterparts. In situ CO-DRIFTS, XPS, and kinetic experiments demonstrate that the electron interaction between Rh and Co atoms effectively lowers the apparent activation energy, thus promoting the tandem hydroformylation/hydrogenation reaction. This work not only presents a novel tandem hydroformylation/hydrogenation reaction system for converting olefins to alcohol but also throws light on the rational design of versatile bifunctional catalysts for ondemand synergistic catalysis.

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含油污泥基材料的制备及应用研究进展

化工新型材料 2024年第S1期52卷 32-36页

作者：王健季宏兵北京科技大学能源与环境工程学院北京100083

含油污泥是石油工业生产过程中产生的危险固体废物,具有复杂的成分和潜在的毒性危害。为解决其环境影响,资源化处理成为主要研究方向。热解技术因其高效处理有机物的优点备受瞩目,其产物可作为化工原料回收利用,具有广泛应用前景。影响... 详细信息

含油污泥是石油工业生产过程中产生的危险固体废物,具有复杂的成分和潜在的毒性危害。为解决其环境影响,资源化处理成为主要研究方向。热解技术因其高效处理有机物的优点备受瞩目,其产物可作为化工原料回收利用,具有广泛应用前景。影响功能性材料制备的工艺参数包括热解温度、时间和升温速率,其优化可显著提升材料性能。共热解、活化改性等方法也为基材料性能的提升提供了有效途径。含油污泥基功能性材料在吸附、催化和电化学领域具有广阔的应用前景,将为环保和资源化利用提供新的解决方案。

关键词：含油污泥热解功能性材料资源化利用

外放疗联合仑伐替尼和卡瑞利珠单抗治疗不可切除肝癌的疗效与安全性评价

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中国肿瘤 2024年第5期33卷 420-427页

作者：季洪兵潘建基刘文晖福建医科大学孟超肝胆医院福建福州350028 福建省肿瘤医院福建福州350014

[目的]评价外放疗联合仑伐替尼和卡瑞利珠单抗治疗不可切除肝细胞癌(HCC)的疗效和安全性。[方法]回顾性分析福建医科大学孟超肝胆医院2018年5月1日至2021年3月1日收治85例不可切除的HCC病例,30例不可切除的HCC患者纳入外放疗联合仑伐替... 详细信息

[目的]评价外放疗联合仑伐替尼和卡瑞利珠单抗治疗不可切除肝细胞癌(HCC)的疗效和安全性。[方法]回顾性分析福建医科大学孟超肝胆医院2018年5月1日至2021年3月1日收治85例不可切除的HCC病例,30例不可切除的HCC患者纳入外放疗联合仑伐替尼和卡瑞利珠单抗组(RT+LC),55例纳入仑伐替尼和卡瑞利珠单抗组(LC)。主要研究终点为无进展生存期(PFS)和总生存期(OS)。次要研究终点包括根据改良的实体肿瘤反应评估标准评估肿瘤治疗反应,以及采用不良事件通用术语标准5.0评估的治疗相关不良事件(TRAEs)。采用单因素和多因素Cox回归分析来确定独立的预后因素。[结果]RT+LC组和LC组的中位PFS分别为11.61个月和7.25个月(P=0.036)。RT+LC组和LC组的中位OS分别为20.07个月和12.03个月(P=0.019)。Cox回归分析显示,联合RT是PFS和OS的独立因素(P均0.05),安全性相当。[结论]外放疗联合仑伐替尼和卡瑞利珠单抗治疗不可切除HCC临床效果显著,不良反应可控,是一种安全、有效的治疗方法。

关键词：肝细胞癌放射治疗仑伐替尼卡瑞利珠单抗

Pt-Ga/CeO_(2)-ZrO_(2)-Al_(2)O_(3)脱氢裂解双功能催化剂用于正丁烷催化制烯烃研究

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化工学报 2024年第5期75卷 1855-1869页

作者：莫锦洪韩雪朱毅翔李菁王旭裕纪红兵广西大学化学化工学院广西南宁530004 江苏科技大学环境与化学工程学院江苏镇江212100 浙江工业大学化学工程学院/浙江绿色石化与轻烃转化研究院/绿色化学合成技术国家重点实验室培育基地浙江杭州310014

正丁烷分子结构相对稳定,C-C键键能较高,难以有效利用,目前大部分作为低价值燃料,通过脱氢、裂解等反应将正丁烷转化为高附加值的轻烯烃研究具有重要的科学意义。采用分步浸渍法将Pt和Ga负载到CeO_(2)-ZrO_(2)-Al_(2)O_(3)(CZA)载体制备... 详细信息

正丁烷分子结构相对稳定,C-C键键能较高,难以有效利用,目前大部分作为低价值燃料,通过脱氢、裂解等反应将正丁烷转化为高附加值的轻烯烃研究具有重要的科学意义。采用分步浸渍法将Pt和Ga负载到CeO_(2)-ZrO_(2)-Al_(2)O_(3)(CZA)载体制备PtGa/CZA催化剂,将Pt-Ga_(2)O_(3)引入作为脱氢位点进行脱氢反应(C4H10→C=4),CZA作为酸位点进行裂解反应(C=4→C=3,C=2),同时PtGa与CZA协同提高表面吸附氧含量降低正丁烷活化温度。结果表明,与负载单Pt或Ga催化剂相比,将Pt和Ga同时负载到CZA载体上,可极大提高反应的转化率和选择性,在500℃时,PtGa/CZA催化剂的正丁烷转化率为64.3%,比Pt/CZA和Ga/CZA催化剂分别高55.9%和53.9%,三者轻烯烃选择性均在95%以上。将PtGa/CZA催化剂制成涂层催化剂,提高了正丁烷转化率和催化剂稳定性。PtGa/CZA催化剂优异的活性归因于较低的Ce^(4+)还原温度和表面吸附氧脱附温度、较多的表面吸附氧位点含量和强酸位点含量。

关键词：烷烃催化裂解铂镓催化剂载体

铁基生物炭复合材料修复重金属污染的研究进展

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化工新型材料 2024年第10期52卷 61-65页

作者：钟鑫莲王梦璐季宏兵北京科技大学能源与环境工程学院北京100083

生物炭已被广泛应用于修复重金属污染水体与土壤,但其催化性能较差、芳香性较低、吸附点位较少等不足限制了其应用。由铁基化合物和生物炭制备的铁基生物炭复合材料,在优化生物炭性能的同时,能够很好地改善铁基材料易氧化和易团聚的缺点... 详细信息

生物炭已被广泛应用于修复重金属污染水体与土壤,但其催化性能较差、芳香性较低、吸附点位较少等不足限制了其应用。由铁基化合物和生物炭制备的铁基生物炭复合材料,在优化生物炭性能的同时,能够很好地改善铁基材料易氧化和易团聚的缺点,表现出良好的重金属钝化效果。综述了铁基生物炭复合材料的分类及制备方法,以及该材料对环境重金属污染修复的研究进展,最后指出了铁基生物炭复合材料在实际应用中可能存在的问题。以期为铁基生物炭复合材料在重金属污染修复中的应用提供理论依据。

关键词：生物炭铁基材料铁基生物炭重金属污染环境修复

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Effective implementation and improvement of fast labeled multi-Bernoulli filter

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Journal of Systems Engineering and Electronics 2023年第3期34卷 661-673页

作者： CHENG Xuan ji hongbing ZHANG Yongquan School of Electronic Engineering Xidian UniversityXi’an 710071China

Effective implementation of the fast labeled multi-Bernoulli(FLMB)filter is addressed for target tracking with interval ***,a sequential Monte Carlo(SMC)implementation of the FLMB filter,SMC-FLMB filter,is derived based on generalized likelihood function ***,a box particle(BP)implementation of the FLMB filter,BP-FLMB filter,is developed,with a computational complexity reduction of the SMC-FLMB ***,an improved version of the BP-FLMB filter,improved BP-FLMB(IBP-FLMB)filter,is proposed,improving its estimation accuracy and real-time performance under the conditions of low detection probability and high *** results show that the BP-FLMB filter has a great improvement of the real-time performance than the SMC-FLMB filter,with similar tracking *** with the BP-FLMB filter,the IBP-FLMB filter has better estimation performance and real-time performance under the conditions of low detection probability and high clutter.

关键词： multi-target tracking interval measurements fast labeled multi-Bernoulli(FLMB)filter sequential Monte Carlo(SMC)implementation box particle(BP)implementation