DOI: 10.5061/dryad.6wwpzgncd
title: Janus Mn single atoms for triggering efficient photothermal catalytic CO2 methanation through spin polarization effect

description: Photothermal catalysis, using sunlight as single energy source, is an
 ideal pattern for CO2 reduction. Herein, Mn single atoms (SAs) are
 constructed on the surface of NNSO, which induces spin polarization
 effect, thus promoting directional transfer of photothermal electrons, and
 improving electron density of Mn sites and adsorption ability of CO2.
 Meanwhile, Mn SAs act as new active sites enhancing the adsorption of
 intermediate *CO, thus suppressing CO production, lowering energy barriers
 of hydrogenation and changing the reaction path. Additionally, the
 hydrogen overflow energy barriers decrease under the effect of spin
 polarization, promoting the rapid transfer of active H from Ni atoms to Mn
 SAs. Resultly, the rate of CO2 methanation is 195.7 mmol g−1 h−1 with
 near-unity selectivity, and the catalytic activity of 1.0%Mn/NNSO
 increases by approximately 140 times compared with NNSO. This is the first
 study that spin polarization effect is utilized to achieve efficient
 photothermal CO2 methanation.
description: # Janus Mn single atoms for triggering efficient photothermal catalytic
 CO2 methanation through spin polarization effect Dataset DOI:
 [10.5061/dryad.6wwpzgncd](https://doi.org/10.5061/dryad.6wwpzgncd) ##
 Description of the data and file structure This is the raw data of
 adz7504, including all the figures and related data in the main text, as
 well as the data in Supplementary Materials. The raw data mainly includes
 catalytic performance related data and test characterization, etc. ###
 Files and variables #### Usage notes: TThe following is a list of the
 different data types by file suffix included in this repository along with
 brief descriptions for how to work with them. .csv: CSV (Comma-Separated
 Values): A universal format for storing tabular data in plain text, with
 values separated by commas and the first row typically containing column
 headers. It can be directly opened and edited using spreadsheet software
 like Excel or Google Sheets, or viewed in text editors, and is suitable
 for data exchange and simple data storage. Overview of Raw Data CSV.
 Sheets This document provides an overview of the experimental data
 contained within the accompanying Excel file(s). The data spans three key
 dimensions: catalyst performance, structural characterization, and
 reaction mechanism investigation. Below are descriptions of each
 worksheet, including its core information, axis definitions (X and Y), and
 primary use. 1.Catalyst.csv Core Info: Records the photocatalytic
 performance of different catalysts under various conditions, including
 thermal reactions (Heat 100~400 °C), control experiments without light (no
 light), and concentrated sunlight experiments. Entries marked as
 "------" indicate no measurement was taken. X-axis (Columns): A:
 Catalyst Name, B: Light Intensity (W/cm²), C: Space Velocity (mL·g⁻¹·h⁻¹),
 D: CH₄ Yield (mmol·g⁻¹·h⁻¹), E: CO Yield (mmol·g⁻¹·h⁻¹), F: CO₂ Conversion
 (%) Y-axis (Rows): Each row corresponds to a unique set of experimental
 conditions.  2.XRD.csv Core Info:Contains X-ray diffraction data for
 different catalysts and reference samples. Intensity is in arbitrary units
 (a.u.). Format: Every two columns correspond to one sample
 (e.g.,NSO（A&B）, NNSO（C&D）. 1.0%Mn/NNSO(E&F),
 1.2%Mn/NNSO(G&H) , 0.8%Mn/NNSO(I&J) 0.6%Mn/NNSO(K&L)
 1.2%Mn/NNSO(Ni removl)(G&H),Each pair lists the 2θ angle and the
 corresponding diffraction intensity. X-axis (Rows): Diffraction Angle (2θ,
 degrees) Y-axis (Data Columns):Diffraction Intensity (a.u.) 3.EPR.csv Core
 Info: Records the signal intensity of NNSO samples with different Mn
 doping concentrations as a function of the g‑value in Electron
 Paramagnetic Resonance (EPR) spectroscopy. The g‑value reflects the
 resonant magnetic field position and is used to characterize the
 electronic structure and local environment of paramagnetic centers (such
 as Mn ions). X‑axis (Columns): g‑value (dimensionless), corresponding to
 the resonant magnetic field position. Y‑axis (Rows): Signal intensity
 (Intensity, a.u.), reflecting the relative concentration or response
 strength of paramagnetic centers. Sample Columns: Each sample consists of
 a pair of g‑value and intensity columns, totaling five samples:1.0%
 Mn/NNSO (g value & Intensity) NNSO (g value & Intensity) 0.6%
 Mn/NNSO (g value & Intensity) 0.8% Mn/NNSO (g value & Intensity)
 1.2% Mn/NNSO (g value & Intensity) 4.Hgsteresis_loop_plots.csv Core
 Info:Records the magnetization of NNSO samples with different Mn doping
 concentrations as a function of the applied magnetic field, covering a
 wide range from high negative to high positive fields. X-axis
 (Columns):Applied Magnetic Field (Field, kOe) Y-axis (Rows): Magnetization
 (M, emu/g) Sample Columns:1.0%Mn/NNSO(A&B), NNSO(C&D),
 1.2%Mn/NNSO(E&F), 0.8%Mn/NNSO(G&H) 5.CO2_adsorption_.csv Core
 Info: Measures the CO₂ adsorption capacity of NNSO samples with different
 Mn doping concentrations, spanning low to high relative pressure ranges.
 X-axis (Columns): Relative Pressure (P/P₀) Y-axis (Rows): Adsorption
 Amount (cm³/g STP) Sample Columns: Includes 1.0%Mn/NNSO(A&B),
 NNSO(C&D), 0.8%Mn/NNSO(E&F), 1.2%Mn/NNSO(G&H),
 0.6%Mn/NNSO(I&J). 6.CO-TPD.csv Core Info: Measures the CO desorption
 behavior of NNSO samples with different Mn doping concentrations,
 containing numerous temperature-intensity data points. X-axis
 (Columns):Temperature (°C) Y-axis (Rows):Signal Intensity (a.u.) Sample
 Columns:NNSO(A&B), 1.0%Mn/NNSO(C&D), 0.8%Mn/NNSO(E&F),
 0.6%Mn/NNSO(G&H), 1.2%Mn/NNSO(I&J). 7.Dynamic_isotope_study.csv
 Core Info: Investigates the variation in methane formation rate over time
 under two different atmospheres: D₂:CO₂=4:1 and H₂:CO₂=4:1. X-axis
 (Columns):Reaction Time (min) Y-axis (Rows):Methane Formation Rate (rCH₄,
 mol·g⁻¹·h⁻¹) Sample Columns: Columns A & B: D₂:CO₂=4:1 atmosphere;
 Columns C & D: H₂:CO₂=4:1 atmosphere. 8.In_situ_Rama.csv Core
 Info:Tracks spectral changes for NNSO and 1.0%Mn/NNSO at 0, 3, 6, 9, 15,
 20, 25, and 30 minutes of light irradiation. Wavenumbers start from 50
 cm⁻¹ and increase. Format (Columns): Left section (Columns A-P): NNSO
 sample, where every two columns correspond to the wavenumber and intensity
 at a specific time point. Right section (Columns Q-AE): 1.0%Mn/NNSO
 sample, with the same two-column-per-time-point structure. Y-axis
 (Rows):Rows 5 and below contain intensity values corresponding to
 different wavenumbers. 9.In_stiu_infrard.csv Core Info:Records infrared
 spectral data for NNSO and 1.0%Mn/NNSO during 0-30 minutes of light
 irradiation. Wavenumbers start from approximately 650 cm⁻¹. Format
 (Columns):Columns A-R: NNSO sample (every two columns for a time
 point's wavenumber & intensity). Columns S-AE: 1.0%Mn/NNSO sample
 (every two columns for a time point's wavenumber & intensity,
 listed in reverse chronological order). Y-axis (Rows): Absorption
 intensity values for different wavenumbers. 10.FTIR.csv Core Info: Records
 the absorbance of NNSO and 1.0%Mn/NNSO in the mid-infrared region, with a
 wavenumber interval of ~2 cm⁻¹. X-axis (Columns):Column A: Wavenumber
 (cm⁻¹) Y-axis (Rows): Column B: NNSO Intensity (a.u.); Column C:
 1.0%Mn/NNSO Intensity (a.u.) 11.TPSR.csv Core Info: Compares the mass
 spectrometry signal changes for NSO(A&B), NNSO(C&D), and
 1.0%Mn/NNSO(E&F) samples during a temperature-programmed process.
 X-axis (Columns): Columns A, C, E: Temperature (°C) Y-axis (Rows): Column
 B: NSO MS Signal (a.u.); Column D: NNSO MS Signal (a.u.); Column F:
 1.0%Mn/NNSO MS Signal (a.u.) 12.Raman.csv Core Info: Compares Raman
 spectra of NNSO(A&B) and 1.0%Mn/NNSO(C&D) samples, covering a
 wavenumber range from 50 to 3500 cm⁻¹. X-axis (Columns):Column A: NNSO
 Wavenumber (cm⁻¹); Column C: 1.0%Mn/NNSO Wavenumber (cm⁻¹) Y-axis (Rows):
 Column B: NNSO Intensity (a.u.); Column D: 1.0%Mn/NNSO Intensity (a.u.)
 13.CO2-TPD.csv Core Info:Contains duplicate test data for the 1.0%Mn/NNSO
 (A&B) , NNSO (C&D)sample, covering a temperature range from 50 to
 275 °C. X-axis (Columns):Temperature (°C) Y-axis (Rows): Signal Intensity
 (a.u.) 14.UV-VIS.csv Core Info: Presents UV-Vis absorption spectra for
 1.0%Mn/NNSO, NNSO, and NSO samples, covering wavelengths from 200 to 2500
 nm. X-axis (Columns):Wavelength (nm) Y-axis (Rows): Absorbance (a.u.)
 Sample Columns: Every two columns correspond to one sample, in the order:
 1.0%Mn/NNSO(A&B), NNSO(C&D), NSO(E&F).
 15_.Performance_comparison.csv Core Info:Compares the methane yield of
 various catalysts, sorted from highest to lowest yield. X-axis
 (Columns):Column A: Serial Number Y-axis (Rows): Catalyst Name, CH₄ Yield
 (mmol·g⁻¹·h⁻¹) 16.XPS.1.0_Mn-NNSO_Mn2p25℃.csv BE_25.datBinding Energy
 (eV). The x-axis coordinate, used to determine the chemical state of
 elements. CPS_25.dat: Raw Signal Intensity (Counts Per Second). The y-axis
 coordinate, representing the untreated experimental measurement spectrum.
 1_1_25.dat, 1_2_25.dat, 1_3_25.dat: Fitted Peak Components. The fitted
 curve data representing different chemical states after deconvoluting the
 raw spectrum. Background_25.dat: Background Signal. The fitted baseline
 used for subtraction from the raw signal. 17.XPS.1.0_Mn-NNSO_Mn2p120℃.csv
 BE_120.dat: Binding Energy (eV). The x-axis coordinate. CPS_120.dat: Raw
 Signal Intensity (Counts Per Second). The y-axis coordinate, representing
 the untreated experimental spectrum. 1_1_120.dat, 1_2_120.dat,
 1_3_120.dat: Fitted Peak Components. Data for the fitted curves
 representing different chemical states of the Mn 2p spectrum.
 Background_120.dat: Background Signal. The fitted baseline.
 18.XPS.1.0_Mn-NNSO_Mn2p240℃.csv BE_240.dat: Binding Energy (eV). The
 x-axis coordinate. CPS_240.dat: Raw Signal Intensity (Counts Per Second).
 The y-axis coordinate, representing the untreated experimental spectrum.
 1_1_240.dat, 1_2_240.dat, 1_3_240.dat: Fitted Peak Components. Data for
 the fitted curves representing different chemical states (e.g., different
 manganese oxidation states) of the Mn 2p spectrum. Background_240.dat:
 Background Signal. The fitted baseline. 19.XPS1.0_Mn-NNSO_Mn2p360℃.csv
 BE_360.dat: Binding Energy (eV). The x-axis coordinate. CPS_360mn.dat: Raw
 Signal Intensity (Counts Per Second). The y-axis coordinate, representing
 the untreated experimental spectrum. 1_1_360mn.dat, 1_2_360mn.dat,
 1_3_360mn.dat: Fitted Peak Components. Data for the fitted curves
 representing different chemical states of the Mn 2p spectr
 Background_360mn.dat: Background Signal. The fitted baseline.
 20.XPS.1.0_Mn-NNSO_Mn2p.csv BE_Mn 2p/5: Binding Energy (eV). The x-axis
 coordinate. CPS_Mn 2p/5: Raw Signal Intensity (Counts Per Second). The
 y-axis coordinate, representing the untreated experimental spectrum. Mn
 2p_1_Mn 2p/5, Mn 2p_2_Mn 2p/5, Mn 2p_3_Mn 2p/5: Fitted Peak Components.
 Data for the fitted curves representing different chemical states (e.g.,
 different oxidation states) after peak deconvolution of the Mn 2p
 spectrum. Background_Mn 2p/5: Background Signal. The fitted baseline.
 21.XPS.1.0_Mn-NNSO_Ni2P.csv BE_Ni 2p/19: Binding Energy (eV). The x-axis
 coordinate.  CPS_Ni 2p/19: Counts Per Second corresponding to the Ni 2p
 orbital, representing the intensity of detected photoelectron signals,
 which is related to element content and detection sensitivity.  Ni 2p_1~Ni
 2p_6_Ni 2p/19: Peak-fitting data of the Ni 2p orbital (6 sub-peaks in
 total), used to decompose overlapping characteristic peaks in the Ni 2p
 spectrum, corresponding to the signal contributions of Ni in different
 chemical states (e.g., Ni²⁺, Ni³⁺, or states bonded with other elements).
 d. Background_Ni 2p/19: Background Signal. The fitted baseline.
 22.XPS.1.0_Mn-NNSO_O1S.csv BE_O 1s/9: O 1s orbital binding energy  CPS_O
 1s/9: O 1s orbital counts per second (photoelectron signal intensity,
 correlated with O content and detection sensitivity) O 1s_1~O 1s_5_O 1s/9:
 O 1s orbital peak-fitting data (5 sub-peaks, decomposing signals of O in
 different chemical environments) Background_O 1s/9: O 1s orbital
 background signal 23.XPS.after_cycling1.0_Mn-NNSO_Mn2p.csv  BE_Mn 2p/5: Mn
 2p orbital binding energy  CPS_Mn 2p/7: Mn 2p orbital counts per second Mn
 2p_1~Mn 2p_3_Mn 2p/7: Mn 2p orbital peak-fitting data (3 sub-peaks,
 decomposing signals of manganese in different chemical environments)
  Background_Mn 2p/7: Mn 2p orbital background signal
 24.XPS.1.0_NNSO_Ni2p.csv  BE_Ni 2p/19: Ni 2p orbital binding energy CPS_Ni
 2p/19: Ni 2p orbital counts per second (photoelectron signal intensity,
 correlated with nickel content and detection sensitivity)  Ni 2p_1~Ni
 2p_6_Ni 2p/19: Ni 2p orbital peak-fitting data (6 sub-peaks, decomposing
 signals of nickel in different chemical environments)  Background_Ni
 2p/19: Ni 2p orbital background signal 25.XPS1.0_NNSO_O1S.csv BE_O 1s/6: O
 1s orbital binding energy (core XPS index, reflecting the chemical state
 of oxygen)  CPS_O 1s/6: O 1s orbital counts per second (photoelectron
 signal intensity, correlated with oxygen content and detection
 sensitivity) O 1s_1~O 1s_3_O 1s/6: O 1s orbital peak-fitting data (3
 sub-peaks, decomposing signals of oxygen in different chemical
 environments)  Background_O 1s/6: O 1s orbital background signal
 26.XPS.after_cycling1.0_Mn-NNSO_C1S.csv  BE_C 1s/4: C 1s orbital binding
 energy  CPS_C 1s/4: C 1s orbital counts per second (photoelectron signal
 intensity, correlated with carbon content and detection sensitivity)
 C-C_1_C 1s/4: Peak-fitting data for C-C bond in C 1s orbital (one of the
 sub-peaks, corresponding to the signal of single-bonded carbon) C 1s_2_C
 1s/4: Second sub-peak of C 1s orbital (peak-fitting data for other carbon
 chemical states)  C=C_3_C 1s/4: Peak-fitting data for C=C bond in C 1s
 orbital (one of the sub-peaks, corresponding to the signal of
 double-bonded carbon)  C-O_4_C 1s/4: Peak-fitting data for C-O bond in C
 1s orbital (one of the sub-peaks, corresponding to the signal of
 oxygen-bonded carbon) Background_C 1s/4: C 1s orbital background signal
 27.XPS.fresh1.0_Mn-NNSO_C1S.csv BE_C 1s/7: C 1s orbital binding energy
 (core XPS index, reflecting the chemical state of carbon)  CPS_C 1s/7: C
 1s orbital counts per second (photoelectron signal intensity, correlated
 with carbon content and detection sensitivity)  C 1s_1~C 1s_3_C 1s/7: C 1s
 orbital peak-fitting data (3 sub-peaks, decomposing signals of carbon in
 different chemical environments) Background_C 1s/7: C 1s orbital
 background signal 28.XPS.fresh1.0_Mn-NNSO_Mn2p.csv  BE_Mn 2p/5: Mn 2p
 orbital binding energy  CPS_Mn 2p/5: Mn 2p orbital counts per second
 (photoelectron signal intensity, correlated with manganese content and
 detection sensitivity)  Mn 2p_1~Mn 2p_3_Mn 2p/5: Mn 2p orbital
 peak-fitting data (3 sub-peaks, decomposing signals of manganese in
 different chemical environments)  Background_Mn 2p/5: Mn 2p orbital
 background signal ## Code/software The software required for this raw data
 includes CSV. ## Access information Other publicly accessible locations of
 the data: No other accessible location. Data was derived from the
 following sources: The raw data comes from experiments and testing
 analysis.