Chinese Journal of Catalysis ›› 2023, Vol. 54: 188-198.DOI: 10.1016/S1872-2067(23)64523-1
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Pengye Zhanga,1, Wenjin Donga,1, Yuanyuan Zhanga, Li-Nan Zhaoa,b, Hualei Yuana, Chuanjun Wanga, Wenshuo Wanga, Hanxiao Wanga, Hongyu Zhanga, Jian Liua,b,*()
Received:
2023-07-31
Accepted:
2023-09-28
Online:
2023-11-18
Published:
2023-11-15
Contact:
*E-mail: About author:
1Contributed equally to this work.
Supported by:
Pengye Zhang, Wenjin Dong, Yuanyuan Zhang, Li-Nan Zhao, Hualei Yuan, Chuanjun Wang, Wenshuo Wang, Hanxiao Wang, Hongyu Zhang, Jian Liu. Metalated carbon nitride with facilitated electron transfer pathway for selective NADH regeneration and photoenzyme-coupled CO2 reduction[J]. Chinese Journal of Catalysis, 2023, 54: 188-198.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64523-1
Scheme 1. Schematic illustration of photogenerated electron transfer and reaction mechanism of CO2 reduction to HCOO- based on PCNRhbpy4, coenzyme, and immobilized FDH.
Fig. 1. (a) Schematic illustration of catalyst preparation processes. HRTEM images of PCN (b) and PCNbpy4 (c-e). TEM of PCNbpy4 (f) and the corresponding EDS mapping images of C (g), N (h), and Rh (i). XPS curves of survey (j), C 1s (k), N 1s (l), and Rh 3d (m).
Fig. 3. Optical/electrochemical characterization of prepared materials. UV-vis DRS spectra of PCN, PCNbpy4, PCNRhbpy4, and DABP (a), PL (b), TPV (c), and TRPL (d) spectra of PCN, PCNbpy4, and PCNRhbpy4. Photocurrent response measurement (e) and EIS plots (f) of as-prepared catalysts.
Fig. 4. Catalytic performance of as-prepared catalysts. (a) NADH regeneration activities. (b) 1H NMR spectra of the reaction products. (c) The absorbance changes of NADH accompanying the ADH-mediated propanal reduction. (d) Recycling stability tests of PCNRhbpy4. Reaction conditions: 2.5 mg catalysts, 0.1 mol L-1 PBS (containing 15 wt% TEOA, pH = 8) under air condition. (e) The rates of H2 production for different combinations, with the inset showing enlarged view of the red box. (f) The yields of HCOO-. Reaction conditions: 2.5 mg catalysts, 1 U FDH, 0.1 mol L-1 PBS (containing 15 wt% TEOA, pH = 8) under CO2 atmosphere.
Fig. 5. H2 production performance of the catalysts (PCNbpy4 and PCNRhbpy4) with (a) and without (b) NAD+. Reaction conditions: 2.5 mg catalysts, 0.1 mol L-1 PBS (including 15 wt% TEOA, pH = 8) under an N2 atmosphere.
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