The Structure of Monomeric Hydroxo-CuII Species in Cu-CHA. A Quantitative Assessment.

<strong>Data type</strong>: Experimental spectroscopic measurements, computer simulation and analysis Files are with filename extensions: <strong>DSC</strong>, <strong>DAT</strong>, <strong>spc</strong>, <strong>par</strong>, <strong>m</strong>, <strong>f34</strong>,<strong> xyz</strong>, <strong>out</strong>, <strong>in</strong> Information on <strong>origin of the data</strong>: EPR spectroscopic measurements with filename extensions <strong>DSC</strong>, <strong>DTA</strong>,<strong> spc </strong>and<strong> par.</strong> EPR spectroscopic simulation and analyses with filename extension <strong>m</strong>. Periodic DFT computations with(out) filename extensions <strong>out</strong> and <strong>f34</strong> in ASCII format. Molecular cluster computations with filename extensions <strong>in</strong> and <strong>out</strong> in ASCII format. Geometry information of cluster models is stored in <strong>xyz</strong> files in ASCII format. X-band CW-EPR spectroscopic measurements were generated by EMX spectrometer equipped with SHQ cavity produced by Bruker. X-band Pulsed-EPR spectroscopic measurements were generated by ELEXYS 580 EPR spectrophotometer equipped with SHQ cavity and ER035 M NMR gaussmeter produced by Bruker. Periodic DFT computations were generated using distributed parallel version of CRYSTAL17 code. Molecular cluster computations were generated using the ORCA (v4.2.1 and v5.0.2) code. <strong>If the dataset includes multiple files that relate to each other:</strong> Files in <strong>PARACAT_WP3_20220713_01_CW</strong> folder includes X-band CW-EPR spectroscopic measurements; original data are in DTA/DSC and spc/par formats. Files in <strong>PARACAT_WP3_20220713_02_HYSCORE</strong> folder includes HYSCORE spectroscopic measurements; original data are in DTA/DSC formats. Files in <strong>PARACAT_WP3_20220713_03_ESE</strong> folder includes ESE spectroscopic measurements; original data are in DTA/DSC formats. Files in <strong>PARACAT_WP3_20220713_04_MATLAB</strong> folder includes computer simulations/analyses of the EPR measurements; data are in m formats. Files in <strong>PARACAT_WP3_20220713_05_MODELLING </strong>folder includes periodic and cluster quantum chemical computations inputs, outputs and geometries in ASCII format. <strong>Information on</strong>: specialized abbreviations: <strong>EPR</strong> – Electron Paramagnetic Resonance, <strong>CW</strong> – Continuous Wave EPR, <strong>ESE</strong> – Electron Spin Echo detected EPR, <strong>HYSCORE</strong> – HYperfine Sublevel CORrelation spectroscopy, <strong>DFT </strong>– Density Functional Theory, <strong>CCSD</strong> – Coupled Cluster Single Double, <strong>PBEXX</strong> – PBE functional with XX percentage of exact Hartree-Fock exchange, <strong>DSDBLYP</strong> – DSD-BLYP double-hybrid functional, <strong>B3LYP </strong>– B3LYP functional, <strong>DSDPBEP86</strong> – DSD-PBEP86 double-hybrid functional, <strong>CuOH </strong>– CuOH species in Chabazite, zeolite topology, <strong>CuCHA_X </strong>– name of the Copper-exchanged Chabazite sample, <strong>supercell</strong> – indicates the supercell periodic model, <strong>O₂act </strong>– activation of the Chabazite sample in O₂ atmosphere. definitions of variables: <strong>Magnetic field, Temperature.</strong> units of measurement: <strong>Gauss (G), K, degree (°), milliTesla (mT), Hartree (Ha), cm^-1 (ν), megahertz (MHz), nanometers (nm)</strong>. abbreviations: <strong>8mr </strong>is the Cu docking sites; <strong>4c </strong>and <strong>3c</strong> are the different coordination geometry; <strong>OHos</strong> and <strong>OHss</strong> indicate the orientation of –OH group (same side or opposite side with respect to the Al ion). <strong>all </strong>indicates the full periodic frequency calculation of the model. <strong>cluster </strong>indicates the geometry of the cluster model extracted from the relaxed periodic ones. Periodic DFT computations with filename extension <strong>.f34</strong> include structural/symmetry information of optimized structure. Periodic DFT computations without extension contain the input commands. Molecular cluster computations with filename extension <strong>.in</strong>/<strong>.out</strong>/<strong>.xyz</strong> are inputs, outputs, and structure of cluster models.数据类型：实验光谱测量、计算机模拟与分析。所涉文件的扩展名包括：DSC、DAT、spc、par、m、f34、xyz、out、in。 数据来源信息：采用扩展名DSC、DTA、spc及par的文件对应电子顺磁共振（Electron Paramagnetic Resonance, EPR）光谱测量数据；采用扩展名m的文件对应EPR光谱模拟与分析数据；采用ASCII格式、带或不带扩展名.out与.f34的文件对应周期性密度泛函理论（Density Functional Theory, DFT）计算结果；采用ASCII格式、扩展名.in与.out的文件对应分子团簇计算结果；团簇模型的几何信息存储于ASCII格式的xyz文件中。 X波段连续波（Continuous Wave, CW）EPR光谱测量数据由搭载布鲁克（Bruker）生产的SHQ腔的EMX光谱仪采集；X波段脉冲EPR光谱测量数据由搭载布鲁克生产的SHQ腔与ER035 M核磁共振高斯计的ELEXYS 580 EPR分光光度计采集。 周期性DFT计算采用CRYSTAL17代码的分布式并行版本完成；分子团簇计算采用ORCA（v4.2.1及v5.0.2）代码完成。 数据集关联文件说明： PARACAT_WP3_20220713_01_CW文件夹内存储X波段连续波EPR光谱测量数据，原始数据格式为DTA/DSC及spc/par； PARACAT_WP3_20220713_02_HYSCORE文件夹内存储超精细能级相关光谱（HYperfine Sublevel CORrelation spectroscopy, HYSCORE）测量数据，原始数据格式为DTA/DSC； PARACAT_WP3_20220713_03_ESE文件夹内存储电子自旋回波检测EPR（Electron Spin Echo detected EPR, ESE）光谱测量数据，原始数据格式为DTA/DSC； PARACAT_WP3_20220713_04_MATLAB文件夹内存储EPR测量的计算机模拟与分析数据，数据格式为m； PARACAT_WP3_20220713_05_MODELLING文件夹内存储周期性及团簇量子化学计算的输入文件、输出文件与ASCII格式几何信息。 相关说明： 1. 专业缩写： EPR：电子顺磁共振（Electron Paramagnetic Resonance）； CW：连续波EPR； ESE：电子自旋回波检测EPR； HYSCORE：超精细能级相关光谱； DFT：密度泛函理论； CCSD：耦合簇单双激发； PBEXX：含XX比例精确哈特里-福克交换能的PBE泛函； DSDBLYP：DSD-BLYP双杂化泛函； B3LYP：B3LYP泛函； DSDPBEP86：DSD-PBEP86双杂化泛函； CuOH：菱沸石（Chabazite）沸石拓扑结构中的CuOH物种； CuCHA_X：铜交换菱沸石样品的命名； supercell：超胞周期性模型； O₂act：菱沸石样品在氧气气氛中的活化处理。 2. 变量定义：磁场强度、温度。 3. 计量单位：高斯（G）、开尔文（K）、摄氏度（°）、毫特斯拉（mT）、哈特里（Ha）、波数（cm⁻¹，ν）、兆赫兹（MHz）、纳米（nm）。 4. 其他缩写： 8mr为铜配位位点； 4c与3c代表不同的配位几何构型； OHos与OHss表示–OH基团的取向（相对于Al离子同侧或异侧）； all表示对模型进行全周期频率计算； cluster表示从弛豫后的周期性模型中提取的团簇模型几何结构。 补充说明：带.f34扩展名的周期性DFT计算文件包含优化后结构的结构与对称性信息；无扩展名的周期性DFT计算文件为输入命令文件；带.in/.out/.xyz扩展名的分子团簇计算文件分别对应团簇模型的输入文件、输出文件与结构信息。