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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 catalysts.Unlike conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and stability.Furthermore,a volcano curve between Ca addition ratio and catalytic activity is found.Introducing 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

Activity promotion of RhCa/AlOsingle-atom catalyst in1-octene hydroformylation: a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年

作者： Hao Zhang Xingcong Zhang Xilun Wang qingdi sun Hao Liu Hongbing Ji Xiaohui He Huizhou Research Institute Sun Yat-sen University Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research Institute School of Chemistry IGCME Sun Yat-sen University 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

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

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Single Cu atom dispersed on S,N-codoped nanocarbon derived from shrimp shells for highly-efficient oxygen reduction reaction

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Nano Research 2022年第7期15卷 5995-6000页

作者： Hao Zhang qingdi sun Qian He Ying Zhang Xiaohui He Tao Gan Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Recently,Cu-based single-atom catalysts(SACs)have garnered increasing attention as substitutes for platinum-based catalysts in the oxygen reduction reaction(ORR).Therefore,a facile,economical,and efficient synthetic methodology for the preparation of a high-performance Cu-based SAC electrocatalyst for the ORR is extremely desired,but is also significantly challenging.In this study,we propose a ball-milling method to synthesize isolated metal SACs embedded in S,N-codoped nanocarbon(MNSDC,M=Cu,Fe,Co,Ni,Mn,Pt,and Pd).In particular,the Cu-NSDC SACs exhibit high electrochemical activity for the ORR with half-wave potential(E_(1/2))of 0.84 V(vs.reversible hydrogen electrode(RHE),20 mV higher than Pt/C)in alkaline electrolyte,excellent stability,and electrocatalytic selectivity.Density functional theory(DFT)calculations demonstrated that the desorption of OH*intermediates was the rate-determining step over Cu-NSDC.This study creates a pathway for high-performance ORR single atomic electrocatalysts for fuel cell applications and provides opportunities to convert biowaste materials into commercial opportunities.

关键词： ball milling oxygen reduction reaction single-atom catalysis shrimp shell S,N-codoped nanocarbon

Quasi-continuous synthesis of cobalt single atom catalysts for transfer hydrogenation of quinoline

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Chinese Chemical Letters 2022年第5期33卷 2569-2572页

作者： Liyun Huang Hao Zhang Yujie Cheng qingdi sun Tao Gan Qian He Xiaohui He Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute of sun Yat-sen University Huizhou 516216China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China School of Environmental and Chemical Engineering Foshan UniversityFoshan 528000China

Improving the transfer hydrogenation of N-heteroarenes is of key importance for various industrial pro-cesses and remains a challenge so far.We reported here a microcapsule-pyrolysis strategy to quasi-continuous synthesis S,N co-doped carbon supported Co single atom catalysts(Co/SNC),which was used for transfer hydrogenation of quinoline with formic acid as the hydrogen donor.Given the unique ge-ometric and electronic properties of the Co single atoms,the excellent catalytic activity,selectivity and stability were observed.Benefiting from the quasi-continuous synthesis method,the as-obtained cata-lysts provide a reference for the large-scale preparation of single atom catalysts without amplification ef-fect.Highly catalytic performances and quasi-continuous preparation process,demonstrating a new and promising approach to rational design of atomically dispersed catalysts with maximum atomic efficiency in industrial.

关键词： Quasi-continuous synthesis Single atom catalysts Microcapsule Transfer hydrogenation Quinoline

Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

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Science China Chemistry 2020年第6期63卷 810-817页

作者： Qian He Yuying Meng Hao Zhang Ying Zhang qingdi sun Tao Gan Huajian Xiao Xiaohui He Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Institute of Advanced Wear&Corrosion Resistant and Functional Materials Jinan UniversityGuangzhou 510632China Fine Chemical Industry Research Institute School of Chemical Engineering and TechnologySun Yat-sen UniversityZhuhai 519082China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Recently,nitrogen-doped porous carbon supported single atom catalysts(SACs)have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction(ORR)due to their outstanding performance,especially those derived from porphyrin-based materials.However,most of them involve other metal residuals,which would cause the tedious pre-and/or post-treatment,even mislead the mechanistic investigations and active-site identification.Herein,we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin,followed by pyrolysis at high temperature.Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-Nxspecies.Our catalyst shows superior ORR performance with positive half-wave potential(E1/2=0.85 V vs.RHE)in alkaline condition and moderate activity(E1/2=0.68 V vs.RHE)under the acidic condition,excellent methanol tolerance and good long-term stability.All the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.

关键词： single atom catalysts porphyrin precursor-dilution oxygen reduction reaction active site

Synthesis of Nitrogen-doped Carbon Supported Cerium Single Atom Catalyst by Ball Milling for Selective Oxidation of Ethylbenzene

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Chemical Research in Chinese Universities 2022年第5期38卷 1258-1262页

作者： ZHANG Xingcong ZHONG Yunzhu CHEN Hongyu CHENG Yujie sun qingdi ZHANG Hao HE Qian ZHANG Ying GUO Guanghui HE Xiaohui JI Hongbing Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275P.R.China Huizhou Research Institute of sun Yat-sen University Huizhou 516216P.R.China Advanced Energy Science and Technology Guangdong Laboratory Huizhou 516000P.R.China

Through screening Ce precursors and pyrolysis temperatures[Ce(acac)3 as Ce precursors and pyrolysis at 900°C],zeolitic imidazolate framework-8(ZIF-8)derived nitrogen-doped carbon supported cerium single atom catalyst(Ce_(1)/NC)is successfully prepared by ball milling method.The Ce_(1)/NC catalyst exhibits exceptional catalytic performance in the selective oxidation of saturated C―H bonds in aromatic compounds,e.g.,91%conversion and 99%selelctivity can be achieved in the oxidation of ethylbenzene to acetophenone under mild reaction conditions.

关键词： Single atom catalyst Ball milling ZIF-8 Ethylbenzene oxidation

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产品性能关联下绿色设计知识表达及获取方法

中国机械工程 2022年第22期33卷 2717-2726页

作者：柯庆镝孙伯骜薛冰张雷陈鹏飞合肥工业大学机械工程学院合肥230009 江苏徐工工程机械研究院有限公司徐州221004

在大数据、网络化环境中,设计人员无法有效地利用海量的机电产品设计信息与数据来应对当前机电产品全生命周期下绿色设计需求。针对这一问题,提出了基于生命周期性能关联的绿色设计知识表达及获取方法。首先建立基于操作-产品-性能(OPP... 详细信息

在大数据、网络化环境中,设计人员无法有效地利用海量的机电产品设计信息与数据来应对当前机电产品全生命周期下绿色设计需求。针对这一问题,提出了基于生命周期性能关联的绿色设计知识表达及获取方法。首先建立基于操作-产品-性能(OPP)的基本关联构型,提出面向生命周期下绿色设计需求的绿色设计知识表达,并提出该结构内各元素的规范化表达;然后利用同义词林和相似度分析对设计信息及数据进行标注处理,构建基于OPP构型的基础关联词典,提出基于绿色关联度的绿色设计知识获取方法;最后,结合机电产品中液压阀零件实例验证所提方法的有效性。研究结果可实现绿色设计知识的多层次多粒度表达和有效获取,为机电产品全生命周期绿色设计实际应用提供基础方法支撑。

关键词：绿色设计知识表达知识获取生命周期机电产品

Computation of the Magnetic Field and Ripple for the Toroidal Coils in HL-2M Tokamak

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Southwestern Institute of Physics Annual Report 2006年第1期 128-129页

作者： LONG Yongxing MOU Zongze JIAN Guangde sun Aiping YUAN Baoshan GAO qingdi WANG Aike

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微波辅助改性壳聚糖的制备及其絮凝性能

环境工程学报 2016年第12期10卷 6935-6939页

作者：初庆娣朱小梅王巧敏严志宇刘慧孙冰大连海事大学环境科学与工程学院大连116026

以壳聚糖、阳离子醚化剂二甲基二烯丙基氯化铵为原材料,采用微波辐射的方法,制备了壳聚糖接枝共聚物(壳聚糖-二甲基二烯丙基氯化铵),并通过红外光谱分析对改性壳聚糖进行了表征。以接枝率为标准,确定改性壳聚糖的最佳反应条件,并以高岭... 详细信息

以壳聚糖、阳离子醚化剂二甲基二烯丙基氯化铵为原材料,采用微波辐射的方法,制备了壳聚糖接枝共聚物(壳聚糖-二甲基二烯丙基氯化铵),并通过红外光谱分析对改性壳聚糖进行了表征。以接枝率为标准,确定改性壳聚糖的最佳反应条件,并以高岭土悬浊液和实际生活污水作为处理对象,测定了改性壳聚糖的絮凝性能。结果表明,壳聚糖接枝共聚物的最佳制备条件是微波反应温度55℃,反应时间20 min,壳聚糖0.5 g,微波功率270 W,阳离子醚化剂的浓度20%,在此条件下,合成的改性壳聚糖的接枝率为80%。红外光谱分析结果显示,已成功地合成了壳聚糖-二甲基二烯丙基氯化铵接枝共聚物。在絮凝实验中,壳聚糖接枝共聚物的去浊率最高达到91%,COD去除率最高达到77%。其结果表明,壳聚糖接枝共聚物的絮凝性能明显高于原料壳聚糖。

关键词：壳聚糖二甲基二烯丙基氯化铵改性壳聚糖接枝率絮凝性能

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溢油分散剂对原油指纹影响的t检验分析

西安石油大学学报（自然科学版） 2016年第1期31卷 110-115页

作者：王巧敏孙冰初庆娣严志宇刘慧朱小梅于颖大连海事大学环境科学与工程学院辽宁大连116026

以海鸥4号分散剂和华北原油的混合物为对象,采用t检验比较法研究基于诊断比值的油指纹鉴别,旨在考察溢油分散剂对原油指纹的影响。首先,对分散剂及4个油样的GC-FID气相谱图进行比较,表明分散剂的加入会影响原油的谱图;然后,对油样中正... 详细信息

以海鸥4号分散剂和华北原油的混合物为对象,采用t检验比较法研究基于诊断比值的油指纹鉴别,旨在考察溢油分散剂对原油指纹的影响。首先,对分散剂及4个油样的GC-FID气相谱图进行比较,表明分散剂的加入会影响原油的谱图;然后,对油样中正构烷烃(包括姥鲛烷和植烷)的相对含量分布进行研究,结果显示分散剂的加入改变了原油中正构烷烃(包括姥鲛烷和植烷)相对含量的分布,且影响明显;最后,采用t检验法对两两油样进行鉴别比较,发现添加不同量分散剂的原油与初始原油之间及它们彼此之间的指纹均不一致。诊断比C17/Pr和C18/Ph受分散剂的影响最大,Pr/Ph和C17/C18受分散剂影响较小,而(C23+C25+C27+C29)/(C24+C26+C28+C30)和(C19+C20)/(C19+C20+C21+C22)受分散剂影响最小。因此,溢油指纹鉴定需要考虑分散剂的影响。

关键词：溢油分散剂油指纹 t检验