Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol

Supporting Information
for Small, DOI 10.1002/smll.202304574
Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites
on Carbon Nitride for Selective Photooxidation of Methane into Methanol
Pawan Kumar, Peter Antal, Xiyang Wang, Jiu Wang, Dhwanil Trivedi, Ondřej František Fellner,
Yimin A. Wu, Ivan Nemec, Vinicius Tadeu Santana, Josef Kopp, Petr Neugebauer, Jinguang Hu,
Md Golam Kibria* and Subodh Kumar*

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Electronic supporting information (ESI)
Partial thermal condensation mediated synthesis of high-density
nickel single atom sites on carbon nitride for selective
photooxidation of methane into methanol
Pawan Kumar,1
Peter Antal,2
Xiyang Wang,3
Jiu Wang,1
Dhwanil Trivedi,1
Ondřej František
Fellner,2
Yimin A. Wu,3
Ivan Nemec,2
Vinicius Tadeu Santana,4
Josef Kopp,5
Petr Neugebauer,4
Jinguang Hu,1
Md Golam Kibria,1*
Subodh Kumar2*
1
Department of Chemical and Petroleum Engineering, University of Calgary, 2500 University
Drive, NW Calgary, Alberta, Canada
2
Department of Inorganic Chemistry, Faculty of Science, Palacký University Olomouc, Olomouc
77146, Czech Republic
3
Department of Mechanical and Mechatronics Engineering, Waterloo Institute for
Nanotechnology, Materials Interface Foundry, University of Waterloo, Waterloo, Ontario N2L
3G1, Canada
4
Central European Institute of Technology, Brno University of Technology, Purkyňova 123,
61200 Brno, Czech Republic
5
Department of Experimental Physics, Faculty of Science Palacký University Olomouc 17.
listopadu 1192/12, 77900 Olomouc, Czech Republic
*Email: Md. Golam Kibria (md.kibria@ucalgary.ca); Subodh Kumar (subodh.kumar@upol.cz)
Contents
1.0 Experimental section………………………………………………………………....Page S3
1.1. Reagent and Materials ………………………………………..……………………………...Page S3
1.2. Physico-chemical characterization …………………………………………..……………..Page S3
2.0 Synthesis of materials
2.1 Synthesis of atomically dispersed nickel on carbon nitride (NiCN SA)……………...….Page S8
2.2 Synthesis of graphitic carbon nitride (g-C3N4: CN)………………………………………..Page S8
2.3 Synthesis of Ni single atom catalysts with N-graphenic scaffold (NiNC)……………….Page S9
3.0 Photoelectrochemical studies……………………………………...…………………Page S9
4.0 Photocatalytic methane oxidation into methanol……………………………....…Page S10
Figures
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Figure S1. HR-TEM images and EDX spectra of NiCN SAC …………………….........Page S11
Figure S2. HR-TEM images and EDX spectra of CN……….…………………..............Page S12
Figure S3. N2 adsorption desorption isotherm and pore diameter of NiCN…………...…PageS12
Figure S4. TRPL life time spectra of CN and NiCN……………..……………………...Page S14
Figure S5. Survey and HR-XPS spectra of CN ……………………..……….……….....Page S15
Figure S6. Survey and HR-XPS spectra of NiCN SAC……………………………….....Page S16
Figure S7. EEMS map and C K-edge NEXAFS spectra of CN and NiCN SAC….….…Page S17
Figure S8. (a) FT-EXAFS spectra and fit and (b) WT-EXAFS map of NiO………...….Page S18
Figure S9. EXAFS spectra in k-space (k3
-weighted) and fitting………………………...Page S19
Figure S10. EXAFS spectra in q-space…………………………..…………………..…..Page S20
Figure S11. Structure of NiCN and NiNC and first shell Ni-N bond length…………….Page S20
Figure S12. EIS Nyquist plot of CN and NiCN………………………………………………….Page S22
Figure S13. Electrochemical studies………….……………………………..……….......Page S21
Figure S14. Digital photograph of photoreactor used for the CH4OR to CH3OH…….....Page S23
Figure S15. 1
H NMR of the product without catalyst/H2O2 under AM1.5 irradiation..…Page S24
Figure S16. 1
H NMR of product with CN/250 μL H2O2 under AM1.5 irradiation....…...Page S25
Figure S17. 1
H NMR of product with CN/500 μL H2O2 under AM1.5 irradiation…...…Page S26
Figure S18. 1
H NMR of product with CN/1000 μL H2O2 under AM1.5 irradiation…….Page S27
Figure S19. 1
H NMR of product with CN without H2O2 and AM1.5 irradiation……..…Page S28
Figure S20. 1
H NMR of product with NiCN without H2O2 under AM1.5 irradiation…...Page S29
Figure S21. 1
H NMR of product with NiCN/50 μL H2O2 under AM1.5 irradiation.…....Page S30
Figure S22. 1
H NMR of product with NiCN/100 μL H2O2 under AM1.5 irradiation.…..Page S31
Figure S23. 1
H NMR of product with NiCN/250 μL H2O2 under AM1.5 irradiation.…..Page S32
Figure S24. 1
H NMR of product with NiCN/500 μL H2O2 under AM1.5 irradiation…...Page S33
Figure S25. 1
H NMR of product with NiCN/1000 μL H2O2 under AM1.5 irradiation.…Page S34
Figure S26. 1
H NMR of product with NiCN/1000 μL H2O2 under AM1.5 irradiation….Page S35
Figure S27. TEM and AC-HAADF-STEM images of recycled NiCN………………….Page S36
Figure S28. EPR spectra of the CN experiments without H2O2………………………….PageS37
Table S1. PL lifetime decay components………………………………..………...….….Page S15
Table S2. XPS elemental analysis showing at% of C, N, O and Ni……………………..Page S16
Table S3. EXAFS fitting parameters……………………………………….…..……..….Page S21
Table S4. The yield and selectivity of CH4 oxidation products using various catalysts....Page S22
Table S5. Photocatalytic oxidation of CH4 to oxygenates using various catalysts…...…Page S37

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1.0 EXPERIMENTAL
1.1 Reagent and Materials
Melamine and Nickel (II) acetate tetrahydrate were procured from Sigma Aldrich. HCl and
HNO3 were intended from the Lach–Ner. All other substrates, including organic solvents were
purchased from Sigma Aldrich and used as received without any further purification.
1.2 Physicochemical Characterization
1.2.1 Transmission electron microscopy (TEM)
Microscopic TEM images were obtained by HRTEM TITAN 60-300 with an X-FEG type
emission gun, operating at 80 keV. This microscope is equipped with a Cs image corrector and a
STEM high-angle annular dark-field detector (HAADF). The point resolution is 0.06 nm in TEM
mode. The elemental mappings were obtained by STEM-energy dispersive X-ray spectroscopy
(EDS). For TEM a very dilute aqueous dispersion of the catalyst was deposited on the carbon-
coated copper grid. The recycled TEM images were obtained at an acceleration voltage of 300
kV using an image Cs-corrected transmisson electron microscope (TEM) TITAN Themis 60-300
(Thermo Fisher Scientific, USA). More instrument details can be found here:
https://nano.ceitec.cz/high-resolution-scanning-transmission-electron-microscope-fei-titan-
themis-60-300-cubed-titan/
1.2.2 X-ray diffraction (XRD)
X-ray powder diffraction patterns were measured using a MiniFlex600 (Rigaku Corporation,
Tokyo, Japan) equipped with the Bragg-Brentano geometry, and with iron-filtered Cu Kα1,2
radiation (λ = 1.54056 Å). The angular range of measurement was set as 2θ = 10-80°.

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1.2.3 X-ray photoelectron spectroscopy (XPS)
XPS measurements were carried out using thin films of the developed catalyst deposited on the
carbon tape. XPS surface investigation has been performed on the PHI 5000 Versa Probe II XPS
system (Physical Electronics) with a monochromatic Al-Kα source (15 Kv, 50 W) and photon
energy of 1486.7 Ev. Dual beam charge compensation was used for all measurements. All the
spectra were measured in a vacuum of 1.3 × 10-7 Pa and at a room temperature of 21 °C. The
analyzed area on each sample was a spot of 200 µm in diameter. The survey spectra were
measured with a pass energy of 187.850 eV and an electron volt step of 0.8 Ev, while for the
high-resolution spectra, a pass energy of 23.500 eV, and an electron volt step of 0.2 eV were
used. The spectra were evaluated with the MultiPak (Ulvac – PHI, Inc.) software. All binding
energy (BE) values were referenced to the carbon peak C1s at 284.80 Ev.
1.2.4 Photoluminescence Spectroscopy (PL)
Photoluminescence characterization (PL emission spectra and time-resolved photoluminescence)
were carried out on Cary Eclipse fluorescence spectrometer (Agilent, CA, USA) equipped with
xenon pulse flashlight source.
1.2.5 soft X-rays absorption spectroscopy (sXAS)
The electronic structure and chemical coordination of the materials were determined by X-ray
absorption spectroscopy using synchrotron-based soft X-rays (sXAS). Canadian Light Source
(CLS) synchrotron’s spherical grating monochromator (SGM) beamline (CLS port 11ID-1)
operating in the energy range of 250-2000 eV was used for the sXAS analysis
(https://www.lightsource.ca/facilities/beamlines/cls/beamlines/sgm.php#SpectralRange). For the
measurement, the samples in powder form were deposited on a double-sided carbon tape affixed
to the sample holder. The sample holder was mounted in a vacuum chamber at 45º w.r.t. to the
X-ray beam and detector. The measurements were performed at an ultrahigh vacuum (~10-6
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Torr) at room temperature. The samples were exposed to soft X-rays while keeping the spot size
of 50- and 100-microns with the help of the Kirkpatrick-Baez mirror system. The energy and
numbers of emitted photons were measured using Amptek silicon drift detectors (SDDs) having
an energy resolution of ~100 eV. The partial fluorescence yield (PFY) obtained by the SDD3
detector signal was reported due to their appropriate location. Initially, the sample was scanned
in the energy range of 250 to 2000 eV (ΔE ~5 eV) to perform Excitation-Emission Matrix
Spectroscopy (EEMS) measurements to derive information about each element present in the
sample. The EEMS map was obtained by averaging 10 scans keeping an exposure time of 1 min.
After each measurement, the samples are moved 0.1 mm to avoid any radiation damage. The C
K-edge, N K-edge and Ni L-edge were scanned in an energy window of 100 eV and 10 scans
were averaged to accumulate the final spectra. SGM beamline’s online laboratory acquisitions
and analysis system were used for the data processing to obtain the final EEMS map and near
edge x-ray absorption fine structure (NEXAFS) spectra.
1.2.6 X-ray absorption near edge structure (XANES) and Extended X-ray absorption fine
structure (EXAFS)
The local chemical structure, oxidation state and coordination pattern of the materials were
determined using hard X-rays, X-ray absorption near edge structure (XANES) and Extended X-
ray absorption fine structure (EXAFS) measurement. The Canadian light source’s 06ID-1 Hard
X-ray MicroAnalysis (HXMA) beamline operating in the energy range of 5-40 KeV with a
superconducting Wiggler source and photon flux of 1012
@12 keV was used for the
measurement. The materials were deposited on a Kapton® tape, spread uniformly and mounted
on a hollow plastic holder. The plastic holed with the sample was secured on a sample socket and
irradiated with hard X-rays. The spot size of the X-ray beam was 0.8 mm x 1.5 mm and the
spectral resolution was 1x10-4
. The X-ray energies were calibrated by measuring the energy edge
of a standard sample with one atomic number less than Ni. All the measurements were
performed in transmittance mode between the energy range of 8790-9730 eV. The acquired raw
data were processed, normalized and exported using Athena software.
1.2.7 Synchrotron-based wide-angle X-ray scattering (WAXS)

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The ultrafine crystalline features of the materials were determined using synchrotron-based
wide-angle X-ray scattering (WAXS) measurements performed on a 04ID-1 BXDS-WLE Low
Energy Wiggler Beamline of a Canadian light source. The BXDS/WLE beamline energy range
was 7-22 keV, with a photon flux intensity of 1 x 1012
to 5 x 1012
photons/s in focus on the
sample at 250 mA ring current. The X-ray spot size was 150 μm vertical x 500 μm. Other
parameters were as follows: resolution: ΔE/E, Si (111): 2.8 × 10-4
at 7.1 keV to 6.4 × 10-4
at 15.9
keV. Si (311): 2.5 × 10-4
at 12.9 keV to 4.5 × 10-4
at 22.5 keV, photon energy: 15116 eV (λ =
0.8202 Å) using Si(111) and default detector: Dectris Mythen2 X series 1K. For the
measurement powder samples were deposited on a glass slide kept on a multiple sample holder.
The multiple sample holder can be moved horizontally and vertically by a computer to change
the measurement position. The X-ray wavelength was 0.8202 nm (15116 keV) while the detector
distance was ~170 mm. For the calibration, a standard LaB6 sample was measured first and
obtained Q-1
values were compared with the reported value. The q-1
values d-spacing and other
parameters of the LaB6 sample are also available on the CLS site:
https://brockhouse.lightsource.ca/about/low-energy-wiggler-beamline.[1]
The acquired .xye files
were processed in GSAS-II software to export the spectra and calculate the Q-1
value and d-
spacing.
1.2.8 Fourier-Transform Infrared Spectroscopy (FTIR)
FTIR spectra were measured using a Jasco FT/IR-4700 spectrometer (Jasco, Easton, MD, USA)
in range (400 – 400 cm–1
) by using the attenuated total reflection (ATR) technique on a diamond
plate.
1.2.9 UV-Vis Spectroscopy (UV-Vis)
The diffuse reflectance UV-Vis spectra were performed at room temperature using Cintra 3030
(GBC Scientific Equipment, IL, USA) equipped with an integrating sphere assembly, using
barium sulfate as reference material.
1.2.10 N2 adsorption desorption measurement
Adsorption/desorption isotherms were measured with N2 at the temperature of liquid nitrogen
(≈77 K) using the adsorption analyser Autosorb iQ-C-MP (Anton Paar QuantaTec, Boyton

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Beach Florida). Prior to the measurement the samples were degassed for 12 h at 60 °C. The
measured data were analysed in ASIQwin software. The BET area was calculated over the P/P0
range determined with Rouquerol´s criteria. The adsorption branch was used for the calculation
of BJH pore size distribution (PSD). The statistical thickness needed for BJH was determined
with the standard method of de Boer.
1.2.11 Elemental analysis
ICP-MS measurements were performed on ICP-MS Agilent 7700x using external calibration.
For fresh samples, a calculated amount of samples was digested and diluted in 50 mL volumetric
flasks, filtered through nylon syringe filter (0.45 µm) and Ni content was determined using ICP-
MS.
1.2.12 Electron Paramagnetic Resonance (EPR)
Room temperature electron paramagnetic resonance (EPR) experiments were conducted using a
JEOL JM-PE-3 resistive magnet and a Magnettech MXH2 microwave source and control unit.
The samples were inserted in a dedicated cuvette to measure liquid samples in polar solvents
(“flat cell”). The flat cell volume within the EPR cavity is 70 uL. The spectra were recorded
using a microwave power of 20 mW and a modulation amplitude of 0.9 G at 100 kHz, in the
magnetic field range of 12 mT centered around 337 mT with a scan time of 60 s.
Samples were prepared with 0.5 mg of catalyst in a total volume of 200 uL. All measurements
were performed with a 20:1 water to methanol ratio. In the experiments with H2O2, the ratio was
also 20:1 of water to H2O2. Irradiation was conducted in situ for the periods indicated in the
results and kept on during the spectra acquisition using a broadband (360 – 2600 nm) light
source SLS201L/M from ThorLabs, with a fiber coupled to its output and a collimator kept 3 cm
away from the sample. According to the typical output power and collimated beam diameter in
the specifications (https://www.thorlabs.com/thorproduct.cfm?partnumber=SLS201L/M), we Formatted: Default Paragraph Font, Font: (Default)
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calculate a irradiance of ~ 20 W m-2
. Control measurements were conducted the same way
except for the absence of the catalyst. The spectra were simulated using the garlic function from
EasySpin (v. 6.0.0-dev.51), a widely used MATLAB package for simulation of EPR data
(Matlab, The Mathworks, Inc., Natick, MA 01760, 2023).[2, 3]
2.0 Synthesis of materials
2.1 Synthesis of atomically dispersed nickel on carbon nitride (NiCN SA)
Melem was synthesized by partial annealing of melamine by a slight modification of the
previous literature method.[4, 5]
Melamine (5.0 g) was taken in a silica crucible covered with a lid
and annealed at 400 °C with a ramping rate of 3 °C min–1
for 2.0 h in a muffle furnace under a
static air atmosphere. Afterward, the prepared melem was cooled down to room temperature and
ground into a fine powder using a mortar pastel. 1.0 g of melem powder was then mixed into 100
mL of distilled water to make a homogenous suspension using sonication for 2 h. In another
beaker, Ni(OAC)2.4H2O (500 mg) was dissolved in 100 mL of distilled water which was then
added dropwise to the melon suspension under vigorous stirring and left the solution overnight.
The resulting mixture was centrifuged, washed and sonicated many times to remove the unbound
nickel acetate and finally freeze-dried to obtain nickel-integrated melon units. The freeze-dried
powder was further calcined at 550 °C under nitrogen for two hours maintaining a heating rate of
3 °C/min and then allowed to cool naturally. The obtained powdered material was treated with
acid solutions (3M HCl and 2M HNO3) to leach out the metallic nickel. Finally, highly dense
atomically dispersed nickel on carbon nitride (Ni-SA-CN) was obtained after washing with water
until neutral pH and drying in a vacuum at 80 °C.
2.2 Synthesis of graphitic carbon nitride (g-C3N4: CN)[6]
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Graphitic carbon nitride was synthesized by thermal annealing of melamine at 550 ºC. In brief, a
silica crucible was charged with 5 g of melamine and covered with a lid. The powder in the
crucible was heated at a ramping rate of 5 °C min-1
up to 550 ºC and kept at this temperature for
4 h. The obtained yellow solid was crushed and ground to make powder for further use.
2.3 Synthesis of Ni single atom catalysts (Ni-N4-C) with N-graphenic scaffold (NiNC)[7]
The Ni single atom catalysts entrapped in N-graphenic carbon (NiNC) was prepared by high
temperature annealing of Ni salt, urea and glucose as reported in literature. In brief, 16.0 g urea
and 1.0 g glucose and nickel acetate, Ni(CH3CO2)2.4H2O (0.276 M) were dissolved in water and
solution was heated at 80 ºC until all water was evaporated. The resulting solid was heated at
900 °C for 5 h to obtain Ni-N4 embedded NiNC catalyst.
3.0 Photoelectrochemical studies
The charge carrier generation performance of the materials was determined by measuring the
photocurrent density of the samples using a three-electrode set-up using 0.1 M Na2SO4 as an
electrolyte. In the three-electrode setup, an anode consisting of a 10 nm TiO2 blocking layer on
FTO glass was coated with carbon nitride materials as assigned as a working electrode.[8]
For
making a slurry, CNs were dispersed in DMF and α-terpineol followed by sonication for 2h and
stirring for another 2h. The obtained slurry was deposited on FTO glass by drop-casting and
heated at 170 ºC to fabricate a thin film. The Pt and Ag/AgCl were assigned as counter and
reference electrodes, respectively. The photocurrent response of the photoanode was measured
under dark and AM1.5 G solar simulated light (HAL-320 Solar Simulator, Class A, 300 W Xe
lamp) with a power density of 100 mW cm-2
at the surface of the sample. The photocurrent
density with respect to time (J-t) was determined at an applied potential of +0.6 V vs Ag/AgCl

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(1.23 V vs NHE; water oxidation potential) during the light on-off cycle. The kinetics of charge-
transfer between materials and electrolyte interface were determined from a Nyquist plot using
Electrochemical impedance spectroscopy (EIS) at an applied bias of –0.5 V vs Ag/AgCl and AC
amplitude of -5 mV at a frequency of 100 kHz. Impedance-potential measurement was
performed to derive the Mott–Schottky plot and calculation of flat band potential. The
measurement was performed in 0.5 M Na2SO4 in a potential range of –1 V to +1 V at 1K
frequency.
4.0 Photocatalytic methane oxidation into methanol
The photocatalytic CH4 oxidation reaction was performed in a custom-made pressure reactor
with a quartz window and gas inlet and outlet. In brief, 10 mg photocatalyst was dispersed in 10
mL of water by ultrasonication, and the suspension was transferred to a photoreactor followed by
the addition of a calculated amount of hydrogen peroxide c.a. 1 mL (30 wt.%). After that, the
reactor was closed and pure CH4 was purged and vented five times to remove any residual gas.
Finally, the reactor was pressurized with 2 MPa CH4. The reactor was irradiated under AM1.5 G
solar simulated light using a class A solar simulator (HAL-320 Solar Simulator, 300 W Xe
lamp). After the reaction, the reactor was cooled at ambient temperature and pressure was slowly
released, and the remaining liquid product was analyzed by 1
H NMR. For the NMR analysis, a
0.5 mL sample was added to the D2O/DMSO mixture (0.1 mL of D2O and 0.05 μL of DMSO).
The water peak suppression was implemented. The quantification was done by adding a known
concentration of possible products as an internal standard.

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Figure S1. HR-TEM images of NiCN SAC at (a-c) 50 nm scale bar showing the nanosheet
structures and (d) at 20 nm scale bar showing the absence of any nanoparticle/nanoclusters and
amorphous nature. (e) EDX spectra display the presence of Ni, C and N in the materials.

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Figure S2. HR-TEM image of CN at (a) 50 nm and (b) 2 nm scale bar.
Figure S3. (a) N2 adsorption desorption isotherm of NiCN shouwing type-II, H3 hysteresis loop
for mesoporous nature (b) BJH pore size distribution of NiCN showing average pore diameter of
2.9 nm.

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Time Resolved Photoluminescence (TRPL)
Photoluminescence (PL) emission corresponds to the recombination of photogenerated
electrons and holes and is useful to understand the efficiency of electron transfer and e−
/h+
pairs separation in the nanocomposites.[40]
Time-resolved photoluminescence (TRPL)
spectra of materials were collected to understand the mechanism of the charge carrier’s
recombination process using a 380 nm excitation (xenon pulse flash lamp) (Figure S4).
The acquired PL lifetime decay curve was fitted tri-exponentially as reported previously
for carbon nitride-based materials using the following equation:
I(t)=A1e-t/τ1
+ A2e-t/τ2
+ A3e-t/τ3
......................................................................................Eq. 1
where, A1, A2 and A3 represent the normalized amplitudes of each decay component and
τ1, τ2 and τ3 are values of the lifetime components, respectively.41,42
The derived lifetime
value and their fractional contributions are listed in Table S1.
The tertiary N-linked heptazine (C6N7) units in carbon nitride constituted alternate C-N
sp2
and C-N sp3
hybridized systems. The sp3
C-N coordination produces high energy σ
and σ* molecular orbital (MO) while π and π* MO resulted from sp2
C-N bonding. Apart
from this, the lone pairs (LP) on secondary nitrogen (:N-C2) can participate in
conjugation, therefore, creating low gap (LP+π) bonding (valence band) and antibonding
(conduction band) hybrid orbital therefore carbon nitride absorbs in the visible region.43,44
The first two shorter lifetime components originated from the direct band-to-band
recombination of (σ*→σ and π*→(LP+π)) excited electrons. Another component with a
relatively larger lifetime originated from the σ*→π* non-radiative intersystem crossing
(ISC) followed by π*→(LP+π) radiative recombination.45–47
Furthermore, low energy
trap sites (defects) mediated recombination also contributes to the third-lifetime

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component.48
Interestingly, after the integration of Ni SA, the value of the third lifetime
was increased drastically suggesting that Ni nanostructures can reduce trap-assisted
recombination due to the ligand to metal charge transfer. Furthermore, the average
lifetime (τavg) which depicts the cumulative recombination process was calculated from
the three-lifetime components using the following equation.
τavg= (A1τ1
2
+A2τ2
2
+A3τ3
2
)/(A1τ1+A2τ2+A3τ3)............................................................. Eq.2
It is clear from Table S1 that the τavg value for CN was found to be (72 μs) which was
increased in NiCN reaching a value of (190 μs) validating the increased lifetime of the
excited species.
Figure S4. Time-resolved PL lifetime spectra of CN (blue dots) and NiCN (red dots). The solid
line represents fitting of the spectra

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Table S1. The PL lifetime decay components and their contribution and calculated average
lifetime (τavg).
Sample 𝝉𝟏 (μs) A1 𝝉𝟐 (μs) A2 𝝉𝟑 (μs) A3 R2 𝝉𝒂𝒗𝒈 (μs)
CN 7.99
1182.4
0
7.95 731.31 94.08 503.94 0.99904 72.47
NiCN 3.47
1549.5
8
3.46
1117.8
8
208.96 463.84 0.98986 190.15
λex: 380 nm
Figure S5. (a) XPS survey scan of CN for elemental analysis. HR-XPS spectra of CN in (b) C1s
(c) N1s (d) O1s regions.

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Figure S6. (a) XPS survey scan of NiCN SAC for elemental analysis. HR-XPS spectra of NiCN
SAC in (b) O1s (c) Na1s (d) Cl2p regions.
Table S2. XPS elemental analysis showing at% of C, N, O and Ni
Sample C (at%) N (At%) O (At%) Ni (At%)
CN 38.22 53.78 8.01 -
NiCN 34.92 35.20 26.50 3.36

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Figure S7. EEMS map for C K-edge region of (a) CN (b) NiCN SAC (c) C K-edge NEXAFS
spectra of CN (black) and NiCN SAC (red).

S18
Figure S8. (a) FT-EXAFS spectra and fit and (b) WT-EXAFS map of NiO

S19
Figure S9. EXAFS spectra in k-space (k3-weighted) and fitting for (a) Ni foil (b) NiO (c) NiNC
(d) NiCN

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Figure S10. EXAFS spectra in q-space. Lower to the upper panel: Ni nitrate, Ni foam, NiNC
and NiCN SAC
Figure S11. Structure of (a) NiCN (b) NiNC showing first shell coordination Ni-N bond length

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Table S3. The EXAFS fitting parameters show coordination number (CN) and bond length.
S. No. Sample bond Bond length (Å) CN E 2 (10-3) R-factor
1 Ni foil Ni-Ni 2.48 12* 5.96 (0.4) 6.0 (0.4) 0.001
2 NiO Ni-O 2.13 5.95 3.2 (0.3) 9.1 (0.7) 0.020
Ni-Ni 2.97 11.94 1.8 (0.2) 5.5 (0.6)
3 NiCN Ni-N 1.90 1.79 8.7 (0.9) 9.7 (0.7) 0.006
Ni-N 2.00 2.14 9.3 (0.8) 9.4 (0.9)
4 NiNC Ni-N 1.97 2.08 9.8 (0.8) 8.8 (0.9) 0.008
Figure S12. EIS Nyquist plot of CN (black) and NiCN (red)

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Figure S13. Mott-Schottky plot of CN (black) and NiCN (red).
Table S4. The yield and selectivity of CH4 oxidation products using various catalysts.
Catalysts H2O
2
(μL)
Time
(h)
Irradiati
on
CH3O
H
CH3OO
H
OHCH2OO
H
HCOOH Total
Oxygena
tes
CH3OH
selectivity
NiCl2 1000 2 Yes - - - - - -
NiO 1000 2 Yes 263 348 - - 611 43
NiNC 1000 2 Yes - - - - - -
CN - 2 Yes 24 - - - 24 -
CN 1000 2 No - - - - - -
CN 250 2 Yes 295 680 63 0 1038 28
CN 500 2 Yes 284 1485 0 0 1769 16
CN 1000 2 Yes 193 3002 580 870 4645 4
NiCN - 2 Yes 116 - - - 24 100
NiCN 1000 2 No - - - - - -
NiCN 50 2 Yes 270 1719 0 0 1989 14
NiCN 100 2 Yes 454 1603 0 0 2057 23
NiCN 250 2 Yes 1591 0 0 0 1591 100
NiCN 500 2 Yes 1580 242 0 0 1822 87
NiCN 1000 2 Yes 1032 485 385 0 1092 94

S23
Figure S14. Digital photograph of photoreactor used for the CH4 oxidation to CH3OH.

S24
Figure S15. 1
H NMR spectra of CH4 oxidation reaction product in the absence of catalyst and
H2O2 under AM1.5G irradiation.

S25
Figure S16. 1
H NMR spectra of CH4 oxidation reaction product using CN as catalyst, under
AM1.5 solar irradiation with 250 μL H2O2.

S26
Figure S17. 1

S27
Figure S18. 1

S28
Figure S19. 1
H NMR spectra of CH4 oxidation reaction product using CN as a catalyst, without
irradiation and H2O2.

S29
Figure S20. 1
H NMR spectra of CH4 oxidation reaction product using NiCN SAC as a catalyst,
under AM1.5G irradiation and without H2O2.

S30
Figure S21. 1
under AM1.5G irradiation and 50 μL H2O2.

S31
Figure S22. 1

S32
Figure S23. 1

S33
Figure S24. 1

S34
Figure S25. 1

S35
Figure S26. 1
H NMR spectra of CH4 oxidation reaction product using NiO as a catalyst, under
AM1.5G irradiation and 250 μL H2O2.

S36
Figure S27. (a-b) TEM images of recycled NiCN catalysts at 20 nm scale showing absence of
any nanoparticulate structure. (c-d) AC-HAADF-STEM images of recycled NiCN catalysts
showing presence of isolated Ni sites and demonstrate absence of any nanoparticles/nanoclusters.

S37
Figure S28. EPR spectra of the CN experiments without H2O2. Simulation parameters: aN =
1.57 mT, aH = 2.32 mT, peak-to-peak linewidth 0.17 mT (assigned to carbon based DMPO
adducts) Conditions: 0.5mg catalyst, H2O:MeOH (20:1) 200uL, 200mM DMPO
Table S5. Photocatalytic oxidation of CH4 to oxygenates using various single atom and
nanoparticulate catalysts.
Single atom Photocatalysts
S.
No.
Photocatalyst (SA
metal content)
Pressure Light
Source
Oxidan
t
Yield (%) Sel. (%) Ref.
1. W-SA-PCN
SAPs (0.47 wt%)
0.5 MPa
CH4
300 W Xe
lamp
H2O C1 products-4956 µmol gcat
−1
CH3OH-1076 µmol gcat
−1
in 5
h.
- [9]
2. PMOF-RuFe(OH)
(2.6 wt%)
1 atm CH4 Xe lamp
(400–
780 nm)
H2O
and O2
CH3OH-
3145 ± 340 µmol gcat
−1
h−1
CH3OH-98% [10]
3. Au1/In2O3 (0.10
wt%)
20 bar CH4 Xe lamp
(300–1100
nm)
10 bar
O2
HCHO-5.95 mmol g–1
after 3h HCHO-
97.62%
[11]
4. Au1/BP (0.2 wt%) 30 bar CH4 Xe lamp H2O CH3OH-113.5 μmol gcat
−1
CH3OH-99% [12]
5. Pd-def-In2O3 (0.083
wt%)
9 bar CH4 LED lamp
(420 nm)
O2 C1 products-179.7 μmol after
3h
CH3OOH-107.6 μmol
CH3OH-37.9 μmol
C1 Select.-
80.4%
[13]

S38
HCHO- 34.3 μmol
6. Rh1/pMOF (5.04 wt
%)
15 bar CH4 AM 1.5G
(100
mW/cm2
)
4 bar
O2, 5
bar CO
CH3COOH-1.42 mmol
CH3OH - 0.11 mmol
HCOOH-0.17 mmol after 3h
CH3OH-65.0% [14]
7 AC-Co1/
PCNKOH
8 bar CH4 Xe lamp
(300–780
nm)
H2O/C
H3CN
CH3OH-355.25 mmol after 6h CH3OH-
87.22%
[15]
8 (Pt/NPW)/TiO2 (1
wt %)
8 bar CH4 400 W Hg–
Xe lamp
1 bar
CO
CH3COOH-118.5 μmol gcat
–1
after 4 h
CH3COOH-
78%
[16]
9 Au1/WO3 (0.1 wt%) 2.0 MPa
CH4
300 W Xe
lamp
(> 420 nm)
H2O2 CH3OH-589 µmol g−1
h-1
HCHO- 10 µmol g−1
h-1
CH3OH-75% [17]
10 Pd1/2DT 20 bar CH4 300 W Xe
lamp (>
420 nm).
H2O2 CH3OH-175 μmol g–1
CH3OH-94 [18]
11 Ni−NC/TiO2 (0.5
wt %)
2 MPa
CH4
300 W Xe
lamp (300
nm < l < 500
nm)
0.1
MPa
O2
C1 oxygenates-198 μmol for 4
h
CH3OOH-55 μmol
CH3OH-29 μmol
HCHO-114 μmol
C1 select.-93% [19]
12 Pd/H-TiO2
nanocages
(0.52 wt%)
2 MPa
CH4/O2
(98:2)
300 W Xe
lamp
O2 CH3OH 4.5 mmol/g/h CH3OH-70% [20]
Nanoparticulate Photocatalysts
14 q-BiVO4 10 bar CH4 Hg lamp
(300–
600 nm)
10 bar
O2
CH3OH-2.3 mmol g−1
HCHO-1.9 mmol g−1
after 7h
CH3OH -
59.7 HCHO-
21.3%
[21]
15 TiO2/OB3b CH4 and
O2 1:1
Xe lamp O2 CH3OH-15,761 ± 142 μmol
g−1
h−1
CH3OH-100% [22]
16 Cu/CeO2 1.2 MPa
CH4
300 W Xe
lamp
1.2
MPa
CO2
CH3OH-88.9 μmol g–1
h–1
CH3OH-95%. [23]
17 Cu–W–TiO2 2 MPa
CH4
300 W Xe
lamp (350 ≤
λ ≤ 760 nm)
0.2
MPa
O2
C1 oxygenates-34.5 mmol g–1
C1 selectivity-
97.1%
[24]
18 BiVO4/V2O5 CH4/He
(20%) gas
mixture
sparged
450 W Hg
lamp
NO C1 oxygenates-10.7 μmol h–1
g–1
C1 selectivity-
100%
[25]
19 0.1 wt % Au/ZnO 2 MPa
CH4
300 W Xe
lamp (300-
500 nm)
0.1
MPa
O2
C1 oxygenates-125 μmoles h-1
C1 selectivity-
95.4
[26]
20 Au–Pd/TiO2 3.0 MPa
CH4
Xe lamp
(>425 nm)
1.0
MPa
O2
C1 oxygenates-20.0 mmolg−1
CH3OH-12.6 mmol gcat
−1
in 1h
C1 selectivity-
98%
[27]
21 Keggin-type POMs
on TiO2
3 MPa
CH4
300 W Xe
lamp
2 MPa
O2
C1 oxygenates-1359 μmol
gcat
−1
C1 selectivity-
82.4
[28]
22 TiO2{001})-C3N4 1 atm CH4 300 W Xe
lamp
H2O2 HCOOH-
486 μmol gcatalyst
−1
h−1
HCOOH-
97.0%
[29]
23 g-C3N4@Cs0.33WO3 1000 ppm
of CH4 gas
300 W Xe
lamp
pure air
(O2:N2
=
20:80)
C1 oxygenates-7.50
μmol after 4 h
- [30]
24 SrWO4/TiO2 2 MPa 300 W Xe 0.2 C1 products-13365 μmol g-1
in C1 selectivity- [31]
Formatted: Font color: Auto, Portuguese (Brazil)

S39
CH4 lamp (300–
420 nm)
MPa
O2
2 h 98.7%
25 Bi2WO6/TiO2–P25 CH4 in He
(20%)
sparged
(∼22.4
mL/min)
450 W Xe
lamp
- C1 oxygenates-4.6 μmol h–1
C1 selectivity-
27.6
[32]
26 0.30%
RuOx/ZnO/CeO2
1 mL CH4
gas
300 W Xe
lamp-
λ>320nm
O2 CH3OH-133.54 μmol g–1
h–1
CH3OH-97.7% [33]
27 BiOCl-Ov CH4 (10
%) and N2
(90 %) was
bubbled
500 W Xe
lamp
H2O2 CH3OH-180.75 μmol gcat−1
h−1
CH3OH-80.07
%
[34]
28 S-CTTP-0.10 0.24 MPa Xe lamp H2O2 CH3OH-8.09 mmol g−1 CH3OH-
75.28 %
[35]
29 Au-CoOx/TiO2 2.0 MPa
CH4
300 W Xe
lamp (300–
500 nm)
0.1
MPa
O2
C1 products- (CH3OOH and
CH3OH)-50.8 μmol for 2 h
C1- selectivity-
95%
[36]
30 BiVO4 bipyramids 10% CH4
and 90%
Ar gas
bubbled
350 W Xe
lamp
O2 CH3OH-111.9 μmol h–1
g–1
CH3OH-85.0% [37]
31 WO3/Fe3+ system CH4
(4.5 mL mi
n−1
) and
He
(17.9 mL
min−1
)
purged
quartz
mercury-
vapor lamp
O2 CH3OH-67.5 μmol h−1
g−1
CH3OH sel-
37.4%
[38]
32 Aux/ZnO CH4/O2
15/5 bar
Xe lamp O2 CH3OH-1371 μmol g−1
CH3OH
selectivity-
99.1%
[39]
33 g-CN 30 bar CH4 300 W Xe
lamp
(>420 nm)
H2O2 CH3OH- ∼ μmol gcat
-1
- [40]
34 c-WO3 20 bar CH4 300 W Xe
lamp
O2 HCHO 13.6 μmol g−1
HCHO-100 % [41]
35 {001} TiO2 2 MPa CH4 300 W Xe
lamp
0.1 MP
O2
CH3OH-4.8 mmol g-1
h-1
CH3OH-80% [42]
36 TiO2–P 2.0 MPa-
O2/CH4
300 W Xe
lamp
O2 C1 oxygenates-3080 μmol g–
1
h–1
HCHO- 2309 μmol g–1
h–1
C1 selectivity-
94.2%
[43]
37 WO3/La CH4/He-
4.5 and
17.9 mL m
in−1
sparged
medium-
pressure
mercury
lamp
O2 CH3OH-8.5 µmol h-1
CH3OH-50% [44]
38 GaN 120 mmol
of CH4
under 1
atm
300 W Xe
lamp
0-8 mL
O2
C1 oxygenates- 20.01 mmol g-
1
C1 select.-
90%.
[45]
39 Pd/MoO3 CH4 was
bubbled
300 W Xe
light
H2O2 C1 Oxygenates-42.5 μmol
gcat−1 h−1
C1 select.-
98.6%
[46]
40 A/R-TiO2 20 bar CH4 300 W Xe 5 bar HCHO-24.27 mmol gcat
–1
HCHO-97.4% [47]

S40
lamp (300–
1100 nm)
O2
41 Cu-0.5/PCN (0.37
wt%)
bubbled
CH4-
(10 mL mi
n−1
)
Visible light H2O C2H5OH-106 μmol gcat
−1
h−1
- [48]
42 CePMo/TiO2 3 MPa
CH4
300 W Xe
lamp
2 MPa
O2
C1 oxygenates-5618.5 μmol
gcat
-1
HCOOH-1052.1 μmol gcat
-1
- [49]
43 AuFe-ZnO 18 bar CH4 300 W Xe
lamp
2 bar O
2
CH3OH-1365 μmol g−1
h−1
CH3OH-90.7% [50]
44 Pdx-def-TiO2 2 MPa
CH4
LED lamp
(365 nm)
0.1 MP
O2
C1 oxygenates-
54 693 μmol g−1
h−1
C1 select.-
98.6%
[51]
45 Co3O4/ZnO 1 atm CH4 300 W Xe
lamp
(380 nm-
860 nm)
O2 CH3OH- 366 μmol g-1
h−1
- [52]
46 FeOOH/Li0.1WO3 2MPa CH4 300 W Xe
lamp
H2O2 CH3OH-231 μmol g–1
CH3OH-86% [53]
47 SiW12Ox/TiO2 1atm CH4 300 W Xe
lamp
O2 C1 oxygenates-1459.5 μmol
gcat
−1
HCHO Selec.
HCHO-
68.7 %,
[54]
48 RhB/TiO2 2 MPa
CH4
Xe lamp O2 CH3OH-143 µmol g−1
h−1
Select: 94% [55]
49 cWO3 20 bar-
CH4/O2
Xe lamp O2 HCHO- 4.61 mmol g−1
HCHO-99.4% [56]
50 ZnO nanosheets 1 bar CH4 300 W Xe
lamp >420
nm
H2O2 C1 oxygenates-2.21 mmol g–1
h–1
C1 select.-
90.7%
[57]
51 TiO2@SiO2-AuPd 6.9 bar
CH4
365 nm UV
LED
2.75
bar O2
C1 oxygenates-15.4 mmol gcat
-
1
h-1
C1 select.-
94.5%
[58]
52 Cu2@C3N4
(~0.35 wt%)
1 MPa CH4 300 W Xe
lamp (>
420 nm)
0.5 MP
O2
C1 products-249.7 μmol at 2 h C1
select.>98%
[59]
53 0.1 wt % Au/ZnO 2 MPa
CH4
300 W Xe
lamp (300–
500 nm)
0.1
MPa
O2
C1 oxygenates-250.9 μmol
after 2h CH3OH- 41.2 μmol
CH3OOH-123.4 μmol
HCHO-86.3 μmol
C1 select.-
95.4%
[60]
54 NiCN (3.25at%) 2 MPa
CH4
300 W Xe
lamp
H2O2 CH3OH-1591 μmol g-1
cat after
2h
CH3OH-100% This
work
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Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol