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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Mechanistic insight into the controlled synthesis of metal phosphide catalysts from annealing of metal oxides with sodium hypophosphite

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Nano Research 2022年第12期15卷 10134-10141页

作者： Fanpeng Chen Bohang Zhao Mengyao Sun Cuibo Liu Yanmei Shi Yifu Yu Bin Zhang Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin UniversityTianjin300072China

Understanding and manipulating synthetic progress for precisely controlling the components and defects of nanomaterials is an important and challenging task in materials synthesis and nanocatalysis.Metal phosphides(MPs)have been explored as cheap advanced materials in various catalytic fields.MP materials are usually synthesized through gas-solid phosphorization reaction in a trial-to-error manner,but their formation mechanism and the origin of controlled synthesis remain unclear.Here,we combine in situ thermogravimetrc analysis-mass spectrometry(TG-MS)and quasi-in situ X-ray powder diffraction(XRD)analysis to probe the transformation mechanism from metal oxides(MOs)to MPs during the phosphorization process mediated by hypophosphite.Temperature,time,and the amount of hypophosphite are revealed as the driven forces while oxophilicity and crystallinity as the impeded forces,simultaneously control the component and defect level of a series of MP(M=Ni,Co,W,Mo,and Nb).The as-obtained WO2.9/WP is proved to be an efficient Z-scheme photocatalyst for oxidative coupling of methane with the total C2+production and C2H4 selectivity in C2+products reaching 10.75 pmolg-1 and 98.25%.Our work provides a fundamental understanding of the phosphorization treatment and thereby guides a viable synthetic route to the controlled synthesis of MOx-δ,MP,MOx-δ/MP,and MP/M heterostructured materials.

关键词： phosphorization treatment metal phosphides methodology heterostructure oxygen vacancy photocatalysis

Uncovering the degradation mechanism induced by ion-diffusion kinetics in large-format lithium-ion pouch cells

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能源化学:英文版 2023年第8期83卷 98-105,I0005页

作者： Shi Zhou Xiaohong Zhang Cong chen Ming chen fanpeng Kong Yingjie Qiao Jiajun Wang Key Laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering University Harbin 150001HeilongjiangChina Chongqing Research Institute of Harbin Institute of Technology Chongqing 401135China

Battery electrochemistry in an actual cell is a complicated behavior influenced by the current density,uniformity,and ion-diffusion distance,etc.The anisotropism of the lithiation/delithiation degree is usually inevitable,and even worse,due to a trend of big-size cell design,typically such as 4680 and blade cells,which accelerated a battery failure during repeat lithiation and delithiation of cathodes.Inspire by that,two big-size pouch cells with big sizes,herein,are selected to reveal the ion-diffusion dependency of the cathodes at different locations.Interestingly,we find that the LiCoO_(2) pouch cell exhibits ~5 A h loss after 120 charge-discharge cycles,but a 15 A h loss is verified in a LiNixMnyCO_(1-x)-yO_(2)(NCM) cell.Synchrotron-based imaging analysis indicates that higher ion-diffusion rates in the LiCoO_(2)than that in the LiNixMnyCO_(1-x)-yO_(2)is the determined factor for the anisotropic cathode fading,which is responsible for a severe mechanical issue of particle damage,such as cracks and even pulverization,in the cathode materials.Meanwhile,we verify the different locations at the near-tab and bottom of the electrode make it worse due to the ion-diffusion kinetics and temperature,inducing a spatially uneven electrochemistry in the big-size pouch cell.The findings give an in-depth insight into pouch cell failure and make a guideline for high-energy cell design and development.

关键词： Ah-level lithium-ion pouch cells Cathode materials lon-diffusion kinetics X-ray tomography

Promoting nitric oxide electroreduction to ammonia over electron-rich Cu modulated by Ru doping

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Science China Chemistry 2021年第9期64卷 1493-1497页

作者： Jiangwei Shi Changhong Wang Rong Yang Fanpeng Chen Nannan Meng Yifu Yu Bin Zhang Department of Catalysis Science and Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Institute of Molecular Plus School of ScienceTianjin UniversityTianjin300072China

Electrocatalytic nitric oxide(NO)reduction is a promising strategy to produce ammonia.Developing a facile approach to synthesize efficient catalysts with enhanced NO electroreduction performance is highly desirable.Here,a series of Ru-doped Cu materials are constructed through in situ electroreduction of corresponding metal hydroxides.The optimized Ru_(0.05)Cu_(0.95)exhibits superior electrocatalytic performance for ammonia synthesis by using NO/Ar(1/4,n/n)as the feedstocks(Faradaic efficiency:64.9%,yield rate:17.68μmol cm^(-2)h^(-1)),obviously outperforming Cu counterpart(Faradaic efficiency:33.0%,yield rate:5.73μmol cm^(-2)h^(-1)).Electrochemical in situ Fourier transform infrared(FTIR)spectroscopy and online differential electrochemical mass spectrometry(DEMS)are adopted to detect intermediates and unveil the possible reaction pathway.The downshift of the Cu d-band center induced by Ru doping facilitates the rate-limiting hydrogenation step and decreases the desorption energy of NH_(3),leading to high Faradaic efficiency and yield of ammonia.

关键词： Electrocatalysis NO ammonia synthesis in situ characterizations Ru-doped Cu

Treatment of Microalgae in Ballast Water Using Hydroxyl Radical in Accordance with the D-2 Ballast Water Discharge Standard

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高电压技术 2014年第1期40卷 232-236页

作者： MENG Xiangying chen Cao BAI Mindong SUN Jian MENG fanpeng Institute of Marine Engineering Department of PhysicsDalian Maritime University College of Environment and Ecology Xiamen University

The effect of hydroxyl radical(·OH) on microalgae in ballast water is experimentally investigated. An ?OH plasma generator, which has a thin plate discharge Ag electrode covered by two α-Al2 O3 dielectric layers, is built. The plasma generator is filled with O2 and gaseous H2 O and is powered by a homemade power supply. ?OH radicals are generated by a series of plasma reactions and then dissolved into ballast water to kill microalgae. The maximum density of the killed microalgae is about 11 000 cells per milliliter. At this density, the microalgae are not reactivated at the 48th hour and the 120th hour in the treated ballast waters, and the content of chlorophyll in these microalgae decreases by 100%. The water quality returns to a normal level after 120 hours without secondary pollution of aquatic organisms and environment. These results show that the requirements of the D-2 ballast water discharge standard defined by the International Maritime Organization(IMO) are satisfied with the proposed treatment, and that ·OH is an ideal substance for killing microalgae during ballast water replacement of ships.

关键词：压载水处理排放标准微藻羟自由基等离子体发生器国际海事组织俄亥俄州最大密度

Phosphate imbalance conducting by BPs-based cancer-targeting phosphate anions carrier induces necrosis

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Chinese Chemical Letters 2021年第4期32卷 1550-1554页

作者： Chunmeng Ma Jinlong Zhang Yuan Zhang chen Ma Minrui Ma fanpeng Ran Xiaoyan Liu Haixia Zhang College of Chemistry and Chemical Engineering.Lanzhou University Lanzhou 730000China

As a vital nutrient closely related to the cance r-cells proliferation,phosphate anions have been paid great attention as a promising anticancer agent.Generally,the transport of phosphate anions depends on a protein transport system which is regulated by ion homeostasis regulations.Herein,we designed a reactive anionic nanocarrier based on black phosphorus nanosheets(BPs)and artesunate(ART),which could enter cells through endocytosis to generate phosphate anions,avoiding the regulation of cell homeostasis.The ionic nanocarrier was coated by polydopamine to defend BPs and ART and functionalized by folate(FA)and hyaluronic acid(HA)for targeting factor.With the anchoring groups FA/HA targeted the carrier into cells,polydopamine coating decomposed to expose ART for further generating reactive oxygen species(ROS)in cancer cell microenvironment,providing oxidation conditions.Next,ROS generated by ART makes BPs decompose to phosphate anions with effectively speed,giving rise to the destruction of ion homeostasis to induce necro sis and inhibit the proliferation for cancer cells.In consequence,this research provides novel idea and direction for the ionic carriers and tumor therapeutics.

关键词： Phosphate anions carrier Black phosphorus nanosheets Artesunate Phosphate imbalance Necrosis

Wide pillar roadway retained in the deep high gas coal seam

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International Journal of Mining Science and Technology 2012年第6期22卷 828-831页

作者： Pan Liyou Feng Enhu Zhao Qingshou chen Liqiang Kong fanpeng Institute of Mining Engineering Shandong University of Science and Technology Bao'an Mine Shanxi Coal Transportation and Sales Group Co.Ltd. College of Natural Resources and Environmental Engineering Shandong University of Science and Technology

According to the geological and mining conditions of deep high gas coal seam,this paper established the mechanical model of stope surrounding rock,and analyzed the stress distribution and deformation failure mechanism of working face and coal pillar.The research determined the arrangement mode that adjacent working faces retain wide pillar,and the reasonable support method of roadway that the combined support of roof and grouting combined together.The reasonable time of reinforced roadway was determined.Through analyzing the mechanical model of the ways of roadway supporting,this research drew the conclusions as follows:the combined support of roof and working slope improved the support strength and range of surrounding rock,optimized the support by adjusting the angle of anchor,and reached the support requirements by using cement grouting in working slope and chemical grout in roof.The technology was applied in 15104 working face of Baoan Mine,and obtained good results.

关键词： Gas Roadway retained Wide pillar Stress distribution Combined support of roof and working slope Grouting

基于BERT与XGBoost的航天科技开源情报分类

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郑州大学学报（理学版） 2021年第3期53卷 15-22页

作者：刘秀磊孔凡芃谌彤童刘旭红北京信息科技大学网络文化与数字传播北京市重点实验室北京100192 北京信息科技大学数据与科学情报分析实验室北京100192 北京跟踪与通信技术研究所北京100192

航天科技开源情报文本内容较长且含有大量专有名词,影响了情报分类的效果,为了提升相关情报的分类准确率,提出一种基于BERT与XGBoost融合模型的航天科技开源情报分类算法。首先通过BERT模型的深度结构提取情报中的关键特征,然后利用XGBo... 详细信息

航天科技开源情报文本内容较长且含有大量专有名词,影响了情报分类的效果,为了提升相关情报的分类准确率,提出一种基于BERT与XGBoost融合模型的航天科技开源情报分类算法。首先通过BERT模型的深度结构提取情报中的关键特征,然后利用XGBoost模型取代BERT最后的输出层,并依据BERT提取到的关键特征对相关情报进行分类。为了验证算法的有效性,设计了与TextRCNN、DPCNN等部分主流语言模型的对比实验,实验结果表明该算法在航天科技开源情报分类中的准确率与TextRCNN、DPCNN模型相比,分别提高了1.9%、2.2%,证明了该算法在相关分类任务中的有效性。

关键词：文本分类 BERT模型 XGBoost模型航天科技开源情报

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基于智能多代理属地管理系统的有序用电模式

电网技术 2019年第5期43卷 1802-1814页

作者：王伊宁丁坚勇田世明卜凡鹏陈俊艺武汉大学电气工程学院湖北省武汉市430072 中国电力科学研究院有限公司北京市海淀区100192

有序用电是缓解供电系统高峰时段供需矛盾的重要手段,随着负荷管理系统的日益智能化,需要充分挖掘用户间的互动能力,提高有序用电决策方案的适用性,为此提出一种包含互济机制在内的智能多代理属地管理系统。在有序用电决策方案中,兼顾... 详细信息

有序用电是缓解供电系统高峰时段供需矛盾的重要手段,随着负荷管理系统的日益智能化,需要充分挖掘用户间的互动能力,提高有序用电决策方案的适用性,为此提出一种包含互济机制在内的智能多代理属地管理系统。在有序用电决策方案中,兼顾用户用电价值、错避峰潜力及其意愿,综合考虑用户与电网的利益,对于居民用户,调整电动汽车充电时段以促进其户用分布式电源就地消纳。并设立动态支援意愿序位表,通过用户间电能互济,对方案做出合理调整。算例分析结果表明了上述方法的有效性和经济性,增强了用户间的互动能力,可实现代理属地内部电力资源自治协调管理。

关键词：有序用电智能代理互济属地管理分布式电源消纳

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电磁场辅助的低温合成氨

Science Bulletin 2023年第17期68卷 1871-1874页

作者：张宝顺王雨婷张娜朱杰伟籍王阳陈凡芃陈星于一夫张兵 Department of Chemistry Institute of Molecular PlusSchool of ScienceTianjin UniversityTianjin 300072China Department of Catalysis Science and Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

近年来,超越传统的氮肥用途,氨越来越多地被认为是一种高密度储能载体和零碳清洁燃料.然而,传统哈伯法合成氨的严苛操作条件极大地限制了氨作为储能载体和燃料的发展.低温下实现氮气高效活化是解决上述问题的关键.本文开发了一种电磁场... 详细信息

近年来,超越传统的氮肥用途,氨越来越多地被认为是一种高密度储能载体和零碳清洁燃料.然而,传统哈伯法合成氨的严苛操作条件极大地限制了氨作为储能载体和燃料的发展.低温下实现氮气高效活化是解决上述问题的关键.本文开发了一种电磁场辅助热催化合成氨新方法.作者采用廉价的商业铁基催化剂作为模型材料,向催化剂床层引入高频、高电压电磁场,使氮气分子的偶极矩和铁基催化剂的电子结构得以被实时调控,进而提高氮气分子在催化剂表面的吸附强度,从而在低温下实现氮气的高效活化.当电磁场存在时,合成氨反应起始温度为100℃,明显低于传统热催化合成氨反应的起始温度(300℃).在填充80 g商业铁基催化剂的放大实验中,相比传统方法,电磁场辅助热催化方法的氨收率提升了5倍、能耗降低了2.7倍.

关键词：铁基催化剂催化剂床层合成氨放大实验起始温度电磁场模型材料偶极矩