Preparation of graphene on Cu foils by ion implantation with negative carbon clusters

We report on few-layer graphene synthesized on Cu foils by ion implantation using negative carbon cluster ions,followed by annealing at 950？C in vacuum. Raman spectroscopy reveals IG/I2 Dvalues varying from 1.55 to 2.38 depending on energy and dose of the cluster ions, indicating formation of multilayer graphene. The measurements show that the samples with more graphene layers have fewer defects. This is interpreted by graphene growth seeded by the first layers formed via outward diffusion of C from the Cu foil, though nonlinear damage and smoothing effects also play a role. Cluster ion implantation overcomes the solubility limit of carbon in Cu, providing a technique for multilayer graphene synthesis.

Solvent-free Synthesis of Flowable Carbon Clusters with Customizable Size and Tunable Optical Performance

We propose a rapid and solvent-flee route for synthesizing luminous carbon clusters by controlling carbonization of polyethylene glycol （PEG）. This approach does not involve solvents yet uses the precursor itself as suspend- ing medium, thus features mild and green chemistry, and also enables the formation of uniform-sized carbon clus- ters, of which the diameter can be easily tuned from 0.7 to 3.5 nm via control of reaction time. In term of the di- mension, the resultants are denoted as sub-nano carbon clusters （SNCs） and carbon dots （CDs）, respectively. Bene- fiting from surface anchored PEG segments, both of the two show favorable flowability at room temperature and excellent solubility in aqueous and organic solvents. Comparison of their optical performances and structures re- veals that they share the same chromophores. Particularly, the SNCs demonstrate robust photo- and pH-stable pho- toluminescence and can be directly applied to cell-imaging regarding to its prominent biocompatibility. Moreover, its quantum yield （5.5%）, which is approximately 3 times higher than that of CDs （1.5%）, can be dramatically en- hanced to 18.8% by facile chemical reduction. We anticipate that these PEG derivatives marked with easy synthesis, controllable optical performances and excellent physical properties will be highly appealing in future applications.

Cluster-assisted generation of multicharged ions in nanosecond laser ionization of carbon bisulfide clusters at 1064nm

The photoionization of seeded carbon bisulfide molecular beam by a 1064nm nanosecond Nd-YAG laser with intensities varying from 0.8 × 10^11 to 5.6 × 10^11 W/cm^2 have been studied by time-of-flight mass spectrometry. Multiply charged ions of S^q＋ （q = 2 6） and C^q＋ （q = 2-4） with kinetic energy of hundreds of electron volts have been observed, and there are strong experimental evidences indicating that those multicharged ions originate from the ionization of CS2 neat clusters in the beam. An electron reeolliding ionization model is proposed to explain the appearance of those multiply charged atomic ions under such low laser intensities.

Molecular dynamics simulation of an argon cluster filled inside carbon nanotubes

The effects of the diameters of single-walled carbon nanotubes （SWCNTs） （7.83A to 27.40A） and temperature （20 K-45 K） on the equilibrium structure of an argon cluster are systematically studied by molecular dynamics simulation with consideration of the SWCNTs to be fixed. Since the diameters of SWCNTs with different chiralities increase when temperature is fixed at 20 K, the equilibrium structures of the argon cluster transform from monoatomic chains to helical and then to multishell coaxial cylinders. Chirality has almost no noticeable influence on these cylindrosymmetric structures. The effects of temperature and a non-equilibrium sudden heating process on the structures of argon clusters in SWCNTs are also studied by molecular dynamics simulation.

Hybridization of Carbon Atomic Orbitals in the Carbon Cluster Cn

In recent years,the stable existence of the C180 has been observed in mass spectroscopy.The existence of C180, C540,…with Ih symmetry can be calculated theoretically, and it has been expected that C540 is a stable construction.

Pseudopotential Density-Functional Calculations for Structures of Small CarbonClusters CN （N=2-8）

We introduce a first-principles density-fumctional theory,i.e.the finite-differcnce pseudopotential density-functional theory in real space and the langevin molecular dynamics annealing technique,to the descriptions of structures and some properties of small carbon clusters(CN,N=2-8).It is shown that the odd-numbered clusters have linear structures and most of the even-numbered clusters prefer cyclic structures.

The Analysis of the Equilibrium Cluster Structure in Supercritical Carbon Dioxide

The monomer fraction density based analysis of precise thermophysical data for pure fluids is developed to study the molecular structures in supercritical fluids in general and in CO2 in particular. The series expansion by powers of the monomer fraction density of the potential energy density is used to discover the cluster structure in supercritical fluids and the clusters’ bond energies in CO2. The method of clusters separation between classes of loose and dense clusters in the CO2 supercritical fluid is developed. The method of the energetically averaged number of dense clusters is developed to study the mechanism of the soft structural transition between the gas-like and liquid-like fluids in the supercritical CO2.

New Method of Generation of Carbon Molecules and Clusters

Firstly the method of joint synthesis of carbon molecules and their hydrides is developed. The stage of high-temperature sublimation of carbon in a new method of generation of carbon molecules is completely excluded. By mass spectrometric method the condensation products of new method of pyrolysis (NMP) benzene are studied. Firstly clusters (C3-C17), typical for carbon vapour, in substances obtained under pyrolysis of hydrocarbons were detected. Fullerene C60 and its hydrides, quasi-fullerenes C48 and C33 inproducts of benzene pyrolysis are detected also. Firstly it is shown what clusters C3-C5 can be generated at so low (100?C-200?C) temperatures of decomposition of substance. Obtained experimental results firstly demonstrate that the small carbon molecules can be generated in reactionary conditions excluding evaporation of carbon. Dehydrogenation and destruction of hydrocarbon molecules is the first stage on a route of the transformation of benzene to carbon molecules.

A QUANTUM CHEMISTRY STUDY ON THE SIZE-DEPENDENCE OF THE CHEMISORPTION OF AMMONIA AND CARBON MONOXIDE ON ALUMINUM CLUSTERS

The chemisorption intensities of NH_3 and CO on aluminum clusters A1_n(n=l-13) have been theoretically predicted by using CNDO/2 method and properly selecting the clusters' geometries.The results show that the chemisorptions of NH_3 and GO on Al_2,Al_6 and Al_12 are magically stable and thus are in good agreement with the experimental results.In addition,an electronic structure analysis is made to expound the nature of such a size effect.

STRUCTURE EFFECTS OF SILICON AND CARBON BY CLUSTER MASS SPECTRA

Microclusters from different structures of silicon and carbon are studied by SIMS under UHV conditions in the mass range below M=200. The sputtered mass spectra of ions Sin+, Cn+ and Cn were obtained from the 10 keV O2+ primary beam bombardment. Comparisons of each spectrum in each group have shown the strong structure effects on the cluster patterns. A brief discussion on the results has been given.

Cluster-Cluster Potentials for the Carbon Nucleus

Two types of potentials are given in the present paper. The two potentials have Gaussian radial dependences. Such shapes of radial functions are suitable for using in the unitary scheme model. The first potential is given in the form of an attractive force and the second is given in the form of a superposition of repulsive and attractive forces. The two potentials are used to calculate the binding energy of the carbon nucleus 12C. For this purpose, we expand the ground-state wave function of carbon in a series of the bases of the unitary scheme model and apply the variational method. To calculate the necessary matrix elements required to obtain the binding energy of carbon, we factorized the unitary scheme model bases in the form of products of two wave functions: the first function represents the set of the A-4 nucleons and the second function represents the set of the last four nucleons by using the well-known four-body fractional parentage coefficients. Good results are obtained for the binding energy of 12C by using the two potentials.

Quantum-Chemical Estimating Interaction of <i>sp²</i>-Carbon Nanoclusters with PE and PP Oligomers

The purpose of this work was to examine the interaction of graphene-like nanoclusters with fragments of polymers of the same nature, but somewhat different structure, for example, polyethylene (PE) and polypropylene (PP) by means of quantum chemistry. By method of density functional theory with the exchange-correlation functional B3LYP, the basis set 6 - 31 G (d, p) and the Grimme’s dispersion correction, the energy values have been calculated of interaction between nanocarbon fragments and oligomers of PE and PP, the most probable structures of their intermolecular complexes being optimized. A graphene-like plane of 40 carbon atoms and 16 atoms of hydrogen was chosen as a model for the surface of the graphene and carbon nanotubes (CNT). In order to take into account the dimensional effect of the surface of the nanotube fragment model on the interaction energy, in addition to the above described, two larger models were used, with the general formula C54H18 and C96N24. It has been found that the interaction energy of nanocarbon fragment with an oligomer of PP is greater, compared with PE, which is consistent with the experimental data on melting temperatures of pure polymers and nanotube-polymer composites. The polymer with a surface of nanocarbon fragment forms an intermolecular complex not bound covalently and retained by intermolecular dispersion forces. Oligomers of polymeric matters and carbon surfaces in formed nanocomplex are placed closer to each other than separate polymeric links between them.

碳中和背景下新疆八大产业的集群发展态势与空间格局研究

不断推进“双碳”目标和特色产业发展是新疆经济社会高质量发展的必由之路.因此,基于2011―2021年新疆八大产业的数据,运用探索性空间数据分析法探究了新疆八大产业的集群发展态势和空间格局,并进一步探讨了碳达峰压力的影响效应.研究表明:1)新疆第一产业占比高于全国平均水平,新疆第二、三产业低于全国平均水平;并且,新疆产业结构高级化低于全国平均水平,产业结构合理化略高于全国平均水平.2)新疆八大产业聚集规模逐渐显现,且位于全国前列.3)新疆八大产业在总量、份额、结构和竞争力上均占据主导地位,是促进区域经济社会发展的优势产业.4)在研究期间内,新疆八大产业对就业和经济增长发挥着重要作用,是地区经济社会发展的重要动力.5)碳达峰压力对新疆八大产业集群发展的影响存在显著差异,有效促进了油气生产加工、绿色有机果蔬和新能源新材料产业的集群发展,但对其它产业集群发展的促进作用还未有效发挥.

基于LMDI和系统聚类的电力行业碳排放影响因素分析

电力行业作为直接使用一次能源的最大部门,是落实我国碳减排目标的重点行业。为厘清电力行业碳排放的主要驱动或抑制来源,论文构建了LMDI模型,从国家及省域两个层面对2006—2020年电力行业碳排放的影响因素进行了分解。研究结果表明,从国家及省域两个层面来看,经济发展效应均为电力碳排放的主要促进因素,火电燃料转化效应和产业结构效应均为电力碳排放的抑制因素,电源结构效应、工业电耗强度效应在全国层面为电力碳排放的抑制因素,但在各省份中的影响效果及程度各有不同。论文以主要抑制因素为变量,利用系统聚类法将30个省份划分为六大区域,针对各区域影响因素的作用效果提出了因地制宜的减排政策。

黄河流域城市群碳足迹及隐含碳转移研究

选择黄河流域5个国家级城市群合计71个城市构建了2017年环境扩展的MRIO模型,评估了包括化石能源燃烧､煤炭开采逃逸､农业非能源排放等3个来源的碳足迹,分析了城市群之间以及城市群内部城市､部门之间的隐含碳转移.结果表明:5个城市群碳足迹总计约2478.34Mt,其中化石能源燃烧贡献了86.42%,是碳足迹的主要来源,煤炭开采逃逸和农业非能源排放亦不容忽视,分别贡献了10.09%和3.49%.煤炭开采和洗选业､金属冶炼和压延加工业､电力热力的生产和供应业是碳足迹的重点部门,生产和消费两个视角下合计分别占总碳足迹的62.67%和36.77%.金属冶炼和压延加工业､电力热力的生产和供应业是隐含碳输出的关键部门,输出量合计占城市群内隐含碳转移量的51.43%,批发零售和住宿餐饮业是输入的关键部门,占比为26.79%,金属冶炼和压延加工业→批发零售和住宿餐饮业是隐含碳主要转移路径.碳足迹和隐含碳转出的重点城市多为资源消耗型､重化工产业占比较高的城市,如鄂尔多斯､滨州等.隐含碳转入的重点城市为维持自身发展需要消耗大量其他城市的产品,如青岛､呼和浩特等.碳足迹主要集中在“几”字弯都市圈､山东半岛和中原城市群,三者碳足迹合计占比在生产和消费视角下分别达到了85.89%和85.02%,“几”字弯都市圈是隐含碳输出最大的城市群,输出量约占城市群间转移量的40.68%,中原城市群是隐含碳输入最多的城市群,输入量约占42.24%.研究结果可为制定和完善黄河流域城市群控碳政策和降碳措施提供更充分合理的依据.

铜纳米颗粒催化剂的重构及其合成碳酸二甲酯性能研究

甲醇氧化羰基化合成碳酸二甲酯(DMC)是中国重点开发的现代煤化工路线,其关键在于高性能催化剂的设计研发。本研究采用液相重构法,通过调变溶剂种类、气氛和压力制得高效铜团簇催化剂,在DMC合成反应中时空收率(STY_(DMC))高达3520 mg/(g·h),经过10次循环,STY_(DMC)下降21.8%。N2吸附-脱附、XRD、TEM、STEM等表征手段表明,强还原性的CO不但可使铜纳米颗粒(~9.7 nm)部分重构为亚纳米团簇(~1.34 nm),同时有效维持了Cu^(0)物种的存在,从而提升了催化活性和稳定性。进一步研究表明,铜重构的发生取决于气氛-金属-载体三者的相互作用,且随氧化、还原性气氛的变化呈可逆状态。

京津冀地区碳排放时空格局变化及其驱动因子

人类对陆地生态系统的改变是碳排放增加的主要原因。在“双碳”目标背景下探索土地利用变化与碳排放的动态关系,有助于区域土地低碳可持续利用。研究基于土地利用转移视角,采用重心-标准差椭圆方法揭示了京津冀地区土地利用碳排放时空格局演化特征,评估了碳排放与生态环境、社会经济发展的协调程度,并借助改进的Kaya模型和LMDI分解模型定量分析了土地利用变化对碳排放的影响程度。结果表明:(1)建设用地的转入是土地利用碳排放增加的主要来源,引起碳排放量增加15844.36万t;耕地、草地向林地、水域的转变促进了地区固碳能力的提升。(2)土地利用碳排放空间分布格局呈现出东北-西南方向向中心进一步聚集的趋势,并且东-西向聚集趋势大于南-北向。(3)京津冀地区整体碳排放与生态环境的协调性呈向好趋势发展,但大部分地区碳排放与社会经济发展出现失衡现象,地区间碳生产力差异逐渐增大。(4)经济水平是促进碳排放增加的最显著因素,单位GDP用地强度是抑制碳排放增加的最主要因素。分析结果表明,严格控制建设用地的无序扩张是促进低碳土地利用的基础,低碳经济发展是促进地区减碳的重要途径。

Growth of C30 and C31 Clusters： Structures, Energetics and Dynamics

We obtain the isomer spectra of C30 and C31 dusters by time-going-backward quasi-dynamics method and perform molecular dynamics simulations of the duster growth from isolated atoms in He buffer gas at 2500 K. The geometrical structures of the isomers of C30 and C31 can be classified into closed cages, open cages, bowls, sheets and other irregular shapes, where closed cages are found to have the lowest potential energies. However, dynamics simulations show that the sheet structures of C30 and C31 are the dominant outcome at the simulation temperature. Compared with relevant experimental results, we propose a different view in interpreting the experimental data and a research procedure to predict isomers that would be formed most probably under specific experimental conditions.

含碳三原子分子结构与电子亲和能的计算

本文分别采用单、双和微扰处理三激发耦合簇方法与自旋非限制的开壳层耦合簇方法对CO_(2),OCS,CS_(2)及其对应阴离子CO_(2)^(-),OCS^(-),CS_(2)^(-)进行高精度的从头算研究.我们计算了这些分子在一系列相关一致基组aug-cc-pV(X+d)Z (X=T,Q,5)以及完全基组极限下的基态平衡几何结构,并研究了芯-价电子相关与标量相对论效应的影响,计算结果与已有文献报道结果吻合较好.基于计算的几何结构,获得了中性分子CO_(2),OCS,CS_(2)的绝热电子亲和能,系统考察了不同基组以及零点能修正对这些分子电子亲和能的影响,给出了考虑各种修正下3种分子准确的电子亲和能.本文将丰富含碳三原子分子的光谱常数和电子亲和能等分子参数的信息,可为实验光谱研究提供重要参考.

基于企业聚类的某省化纤行业节能减碳潜力分析

化纤行业在“双碳”战略目标下面临着巨大的节能减碳压力,需要分析行业的能耗现状与节能减碳潜力。以中国化纤行业第一大省的146家化纤企业为研究对象,利用企业能耗数据分析行业的能耗特征,基于聚类算法对企业进行分类并计算行业的节能减碳潜力。结果表明,该省2013—2021年化纤行业的能耗结构和碳排放结构均以电力贡献为主,节能潜力占行业能耗量的24.63%,减碳潜力占行业碳排放量的22.91%。大型企业和能耗强度偏高的小型企业节能减碳建议以减少原煤消耗为主,中小型企业节能减碳建议以减少电力消耗为主。