Regulating the *OCCHO intermediate pathway towards highly selective photocatalytic CO₂ reduction to CH₃CHO over locally crystallized carbon nitride

Abstract

Locally crystallized PCN is prone to form *OCCHO groups rather than *CH2O groups, regulating the endoergic C–C coupling step to a simultaneous exoergic reaction and changing the reaction pathway towards CH3CHO (selectivity of 98.3%) instead of HCHO.

Insight on Reaction Pathways of Photocatalytic CO2 Conversion

“…As summarized in Table 2 , the benchmark quantum efficiency for C 2 products is 22.4% at 385 nm and 13.3% at 420 nm (CO 2 to acetaldehyde with a 98.3% selectivity) achieved on locally crystallized carbon nitride. 89 Liu et al used DRIFT and theoretical calculation to prove that an amino-2-propanol-assisted hydrothermal treated carbon nitride had strong bonding with the *OCCHO group, which is favorable to a C–C coupling process and changes the reaction pathway to form CH 3 CHO instead of HCHO. The highest quantum efficiency for ethanol was 3.5% on AgBr–N-doped carbon nitride.…”

Atomically Dispersed Au-Assisted C–C Coupling on Red Phosphorus for CO2 Photoreduction to C2H6

“…In recent years, photocatalytic CO 2 conversion has received widespread attention due to its potential application in the production of high-value-added chemicals. , At present, the developed nanoparticle photocatalyst can realize the efficient production of C 1 chemicals such as CO and methane through light-driven CO 2 conversion. , To the best of our knowledge, it is very difficult to produce two-carbon (C 2 ) products in photocatalytic CO 2 reduction because it requires C–C coupling. The formation of C–C bonds needs to overcome a larger reaction energy barrier than the formation of C–H bonds and C–O bonds.…”

“…PR, Pt 1 /PR, Ir1/PR, and Pd1/PR; AC HAADF-STEM image of Au 1 /PR and PR; XPS spectra of P 2p peaks and Au 4f peaks for Au 1 /RP; FTIR and Raman spectra of RP and Au 1 /RP; EXAFS fitting curves of the Au foil at the R space; wavelet-transformed k3 -weighted EXAFS spectra of Au 2 O 3 ; possible structures of Au 1 /RP; photoreduction of CO 2 under various reaction con-ditions; photocatalytic activity of samples in CO 2 reduction reaction and C 2 H 6 evolution rates for RP/ Au x /RP samples; O2 evolution rates of RP and Au 1 /RP samples; standard curve of C 2 H 6 on GC; in situ DRIFTS spectra of Au 1 /RP for CO2 reduction reaction; photocatalytic mechanism of single-atom catalysts; product of isotope-labeled CO 2 experiment; decomposed charge density map for valence band of RP; transient absorption spectrum, PL spectroscopy, UV−vis DRS spectra, and XRD pattern of RP and Au 1 /RP; photocurrent time dependence of RP and Au 1 /RP electrodes under visible light irradiation; EXAFS fitting parameters at the Au L 3 edge for various samples; performance comparison of samples with state-of-the-art catalysts; products formed, selectivity, and relevant reaction conditions; and production evolution rates of Au N /RP and Au 1 /RP samples (PDF) Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510006, P. R. China; orcid.org/0000-0002-7879-6446; Email: huzhf8@mail.sysu.edu.cn Dingsheng Wang − Department of Chemistry, Tsinghua University, Beijing 100084, China; orcid.org/0000-0003-0074-7633; Email: wangdingsheng@mail.tsinghua.edu.cn Yadong Li − Department of Chemistry, Tsinghua University, Beijing 100084, China; College of Chemistry, Beijing Normal University, Beijing 100875, P. R. China; Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, P. R. China; orcid.org/0000-0003-1544-1127; Email: ydli@mail.tsinghua.edu.cn…”

Cu(BF4)2/AC-Catalyzed Synthesis of N-Substituted Anilines, N-Substituted 1,6-Naphthyridin-5(6H)-one, and Isoquinolin-1(2H)-one

“…Finally, the catalyst was further profiled by the Brunauer–Emmett–Teller (BET) method, X-ray diffractometer (XRD), scanning electron microscope (SEM), and X-ray photoelectron spectroscopy (XPS). , Our catalyst has a Brunauer–Emmett–Teller (BET) specific surface area of 675.0 m 2 g –1 . And the pore volume was 0.42 m 3 g –1 (Figure a).…”