Research Article Issue
Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction
Nano Research 2024, 17 (6): 5011-5021
Published: 07 March 2024

Designing catalysts with highly active, selectivity, and stability for electrocatalytic CO2 to formate is currently a severe challenge. Herein, we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO2 reduction reaction. As expected, atomically dispersed In-based catalysts with In-S1N3 atomic interface with asymmetrically coordinated exhibited high efficiency for CO2 reduction reaction (CO2RR) to formate. It achieved a maximum Faradaic efficiency (FE) of 94.3% towards formate generation at −0.8 V vs. reversible hydrogen electrode (RHE), outperforming that of catalysts with In-S2N2 and In-N4 atomic interface. And at a potential of −1.10 V vs. RHE, In-S1N3 achieves an impressive Faradaic efficiency of 93.7% in flow cell. The catalytic performance of In-S1N3 sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure (XANES) measurements under electrochemical conditions. Our discovery provides the guidance for performance regulation of main group metal catalysts toward CO2RR at atomic scale.

Research Article Issue
In situ reconstruction induced oxygen-deficient multiphase Cu based species hybridized with Ni single atoms as tandem platform for CO2 electroreduction
Nano Research 2024, 17 (5): 3888-3894
Published: 29 December 2023

Tandem catalysis, capable of decoupling individual steps, provides a feasible way to build a high-efficiency CO2 electro-conversion system for multicarbons (C2+). The construction of electrocatalytic materials is one of focusing issues. Herein, we fabricated a single atom involved multivalent oxide-derived Cu composite material and found it inclined to reconstruct into oxygen-deficient multiphase Cu based species hybridized with monatomic Ni on N doped C matrix. In this prototype, rapid CO generation and C−C coupling are successively achieved on NiN4 sites and surface amorphized Cu species with defects, resembling a micro-production line. In this way, the in situ formed tandem catalyst exhibited a high Faradaic efficiency (FE) of ~ 78% for C2+ products along with satisfactory durability over 50 h. Particularly, the reconstruction-induced amorphous layer with abundant asymmetric sites should be favorable to improve the ethanol selectivity (FE: 63%), which is about 10 times higher than that of the non-tandem Cu-based contrast material. This work offers a new approach for manipulating tandem catalyst systems towards enhancing C2+ products.

Research Article Issue
Natural keratin-based Fe-S1N3 single atom catalyst for insights into the coordination regulation effect of Fenton-like catalysis with high efficiency
Nano Research 2023, 16 (7): 9003-9011
Published: 02 April 2023

Single atom catalysts (SACs) have attracted great attention, yet the quest for highly-efficient catalysts is driven by the current obstacles of ambiguous structure-performance relationship. Here, we report a nature keratin-based Fe-S1N3 SACs with ultrathin two-dimensional (2D) porous carbon nanosheets structure, by controlling the active center through the precise coordination of sulfur and nitrogen. Compared with natural silk-based Fe-N4 catalyst, the Fe-S1N3 SACs exhibit excellent Fenton-like oxidation degradation ability. X-ray absorption fine structure (XAFS) and electron paramagnetic resonance (EPR) results confirm that S doping is conducive to electron transfer, to accurately generate ·OH with high oxidative degradation capacity at the active site. Therefore, the optimized Fe-S1N3 catalyst showed higher oxidation degradation activity for organic pollutant substrates (methylene blue (MB), Rhodamine B (RhB) and phenol), significantly superior to Fe-N4 samples. This work is devoted to the treatment and application of natural fibers, which provides a novel method for the synthesis of SACs and the regulation of atomic coordination environment.

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