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Controlled Growth of Multidimensional Interface for High-Selectivity Ammonia Production

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CCS Chemistry 2023年第7期5卷 1653-1662页

作者： Xuchen Zheng yurui xue Chao Zhang Yuliang Li CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100190 Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceJinan 250100

The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues.Herein,a new idea has been realized for rational and selective construction of the sp-carbon-metal-carbon interface,comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides,for a highly efficient nitrate reduction reaction.The as-prepared sp-carbon-metal-carbon interfacial structures greatly increase the charge transfer ability and electrical conductivity of the system.The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity,activity,and stability in catalytic system.The catalyst exhibits high Faradaic efficiency of over>95%and a NH3 yield rate up to 205.5μmolNH_(3) cm^(-2) h^(-1) in dilute nitrate conditions without any contaminant.

关键词： graphdiyne donor-acceptor interface incomplete charge transfer high selectivity ammonia production

Ir0/graphdiyne atomic interface for selective epoxidation

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National Science Review 2023年第8期10卷 173-179页

作者： Zhiqiang Zheng Lu Qi Yaqi Gao Xiaoyu Luan yurui xue Feng He Yuliang Li Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringShandong University CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of Sciences School of Chemical Sciences University of Chinese Academy of Sciences

The development of catalysts that can selectively and efficiently promote the alkene epoxidation at ambient temperatures and pressures is an important promising path to renewable synthesis of various chemical products. Here we report a new type of zerovalent atom catalysts comprised of zerovalent Ir atoms highly dispersed and anchored on graphdiyne(Ir0/GDY) wherein the Ir0is stabilized by the incomplete charge transfer effect and the confined effect of GDY natural cavity. The Ir0/GDY can selectively and efficiently produce styrene oxides(SO) by electro-oxidizing styrene(ST) in aqueous solutions at ambient temperatures and pressures with high conversion efficiency of ～100%, high SO selectivity of 85.5%, and high Faradaic efficiency(FE) of 55%. Experimental and density functional theory(DFT) calculation results show that the intrinsic activity and stability due to the incomplete charge transfer between Ir0and GDY effectively promoted the electron exchange between the catalyst and reactant molecule, and realized the selective epoxidation of ST to SO. Studies of the reaction mechanism demonstrate that Ir0/GDY proceeds a distinctive pathway for highly selective and active alkene-to-epoxide conversion from the traditional processes. This work presents a new example of constructing zerovalent metal atoms within the GDY matrix toward selective electrocatalytic epoxidation.

关键词： graphdiyne atom catalyst atomic interface selective epoxidation high-performance

Controlled Growth Interface of Charge Transfer Salts of Nickel- 7,7,8,8-Tetracyanoquinodimethane on Surface of Graphdiyne

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CCS Chemistry 2023年第4期5卷 971-981页

作者： Yuxin Liu Yang Gao Feng He yurui xue Yuliang Li Institute of Chemistry Chinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100

Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne(GDY).The catalytic system of donor–acceptor–donor(GDY/TCNQ/Ni)structure with multiple charge transfer(CT)was achieved by controlling the growth of NiTCNQ on the surface of GDY.Significantly,a controlled double layer interface of GDY/TCNQ/Ni was formed.This system implemented simultaneously the two elements we expected(1)an incomplete CT,and(2)the infinite distribution of active sites originating from highly asymmetric surface charge distribution.The high conductivity and typical semiconductor characteristics of the catalyst endows it with high catalytic activity.We found that an electrolytic cell consisting of the CT salt as a catalyst provided a 1.40 V ultra-small cell voltage up to 10 mA cm−2 and the outer GDY film effectively prevented the corrosion of the catalyst.Our study is the first to introduce CT complexes to a novel catalytic material platform for high selectivity of catalysts,and undoubtedly demonstrates the high selectivity,stability,and activity of such catalytic systems,which provides a new space for the development of novel conceptual catalysts.

关键词： graphdiyne charge transfer salts donor-acceptor-donor structure overall water splitting

2D graphdiyne materials:challenges and opportunities in energy field

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Science China Chemistry 2018年第7期61卷 765-786页

作者： yurui xue Yuliang Li Jin Zhang Zhongfan Liu Yuliang Zhao CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190China Center for Nanochemistry College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China National Center for Nanoscience and Technology Chinese Academy of SciencesBeijing 100190China

Graphdiyne(GDY),a novel two-dimensional(2D)carbon allotrope featuring one-atom-thick planar layers of sp andhybridized carbon network,is a rapidly rising star on the horizon of materials science.Because of its unparalleled structural,electronic,chemical and physical properties,it has been receiving unprecedented increases from fundamental studies to practical applications,particularly the field of energetic materials.In this review,we aim at providing an up-to-date comprehensive overview on the state-of-the-art research into GDY,from theoretical studies to the key achievements in the development of new GDY-based energetic materials for energy storage and conversion.By reviewing the state-of-the-art achievements,we aim to address the benefits and issues of GDY-based materials,as well as highlighting the existing key challenges and future opportunities in this exciting field.

关键词： 2D 精力材料碳同素异形体应用程序地平线电子化学

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Graphdiyne-based metal atomic catalysts for synthesizing ammonia

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National Science Review 2021年第8期8卷 168-177页

作者： Huidi Yu yurui xue Lan Hui Chao Zhang Yan Fang Yuxin Liu Xi Chen Danyan Zhang Bolong Huang Yuliang Li Institute of Chemistry Chinese Academy of Sciences Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong University Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University University of Chinese Academy of Sciences

Development of novel catalysts for nitrogen reduction at ambient pressures and temperatures with ultrahigh ammonia(NH3) yield and selectivity is challenging. In this work, an atomic catalyst with separated Pd atoms on graphdiyne(Pd-GDY) was synthesized, which shows fascinating electrocatalytic properties for nitrogen reduction. The catalyst has the highest average NH3yield of 4.45 ± 0.30 mgNH3mg Pd-1h-1, almost tens of orders larger than for previously reported catalysts, and 100% reaction selectivity in neutral media. Pd-GDY exhibits almost no decreases in NH3 yield and Faradaic efficiency. Density functional theory calculations show that the reaction pathway prefers to perform at the(Pd, C1, C2) active area because of the strongly coupled(Pd, C1, C2), which elevates the selectivity via enhanced electron transfer. By adjusting the p–d coupling accurately, reduction of self-activated nitrogen is promoted by anchoring atom selection, and side effects are minimized.

关键词： graphdiyne atomic catalyst two-dimensional carbon material ammonia nitrogen reduction reaction

Themed Issue on Graphdiyne

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Chemical Research in Chinese Universities 2021年第6期37卷 I0001-I0003页

作者： yurui xue Zicheng Zuo Jin Zhang Yuliang Li Shandong University Institute of Chemistry Chinese Academy of Sciences Peking University

Graphdiyne(GDY)has characteristics of one-atom-thick two-dimensional layers comprising of sp and sp^(2)hybridized carbon atoms.The chemical and electronic structure gives GDY many unique and fascinating properties,such as rich chemical bonds,highly conjugated and super-largeπstructures,infinitely distributed pores and high inhomogeneity of charge distribution,etc.

关键词： infinitely bonds conjugated

Bismuth/Graphdiyne Heterostructure for Electrocatalytic Conversion of CO_(2) to Formate

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Chemical Research in Chinese Universities 2022年第6期38卷 1380-1386页

作者： DU Yuncheng ZHENG Xuchen xue yurui LI Yuliang Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing100029P.R.China Institute of Chemistry Chinese Academy of SciencesBeijing100190P.R.China Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan250100P.R.China School of Chemical Science University of Chinese Academy of SciencesBeijing100049P.R.China

Electrocatalytic CO_(2) reduction is great promising in alleviating the excessive CO_(2) emission and the conversion to valuable productions.Herein we report the in-situ controlled growth of Bismuth nanoflower/graphdiyne heterostructures(Bi/GDY)for efficient CO_(2) conversion toward formate.Based on GDY,the obtained electrocatalyst exhibits a partial current density of 19.2 mA/cm^(2) and high reaction selectivity towards formate with a high Faradic efficiency of 91.7%at−1.03 V vs.RHE,and an energy efficiency of 58.8%.The high formate yield rates could be maintained at around 300µ.mol/(cm^(2)·h)over a wide potential range.Detailed characterizations show that the unique interface structures between GDY and Bi can enhance the charge transfer ability,increase the number of active sites,and improve the long-term stability,and finally reach high-performance electrocatalytic conversion of CO_(2) to formate.

关键词： Graphdiyne(GDY) Heterostructure CO_(2)reduction reaction(CO_(2)RR) Formate

Loading Nickel Atoms on GDY for Efficient CO_(2) Fixation and Conversion

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Chemical Research in Chinese Universities 2022年第1期38卷 92-98页

作者： ZHENG Zhiqiang HE Feng xue yurui LI Yuliang Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100P.R.China Institute of Chemistry Chinese Academy of SciencesBeijing 100190P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

Carbon dioxide(CO_(2))is an important and valuable C1 resource for the synthesis of numerous of value-added products. However, efficient fixation and conversion of CO_(2) into organic carbonates under mild conditions remain great challenges. Herein, graphdiyne(GDY)-based nickel atomic catalysts(Ni0/GDYs) were synthesized through a facile in-situ reduction method. Experimental results showed that the obtained Ni0/GDY had outstanding catalytic performances for converting CO_(2) into cyclic carbonates with a high reaction conversion(99%) and reaction selectivity(ca. 100%) at 80℃ and under 1 atm(1 atm=101325 Pa). Specially, the activation energy (Ea) value for the Ni0/GDY is 37.05 kJ/mol, lower than those of reported catalysts. The reaction mechanism was next carefully analyzed by using density functional theory(DFT) calculations. Such an excellent catalytic property could be mainly attributed to the high dispersion of active sites on the Ni0/GDY, and the unique incomplete charge transfer properties of GDY-based zero-valent metallic catalysts.

关键词： Graphdiyne Atomic catalyst Atomic catalysis CO_(2)fixation CO_(2)conversion

基于多目标优化模型的扇叶最优分组与排列方案

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现代信息科技 2024年第7期8卷 100-106页

作者：薛煌铠宋佳怡苗育睿北京理工大学北京102401

衡量某种机械单片扇叶结构优劣的指标有“质量”与“转动频率”两种参数,为了合理地装配整个风扇,需要相邻组的扇叶质量差达到最小,同时相邻叶片的频率差达到最大。首先构建一个单目标优化的质量分组模型,其后引入递推型动态规划算法,... 详细信息

衡量某种机械单片扇叶结构优劣的指标有“质量”与“转动频率”两种参数,为了合理地装配整个风扇,需要相邻组的扇叶质量差达到最小,同时相邻叶片的频率差达到最大。首先构建一个单目标优化的质量分组模型,其后引入递推型动态规划算法,使得相邻组的扇叶质量差达到最小。同时考虑转动频率的影响,再建立一个多目标优化的质量分组模型,采用动态权重线性加权法,通过对比不同权重下相邻扇叶组的最大质量差和相邻扇叶的最大频率差,发现当A目标和B目标的权重均为0.5时,该模型所给出的方案效果最佳。

关键词：递推型动态规划算法多目标优化分组模型动态权重线性加权法

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