The optimized Fenton-like activity of Fe single-atom sites by Fe atomic clusters–mediated electronic configuration modulation

Abstract

The performance optimization of isolated atomically dispersed metal active sites is critical but challenging. Here, TiO 2 @Fe species-N-C catalysts with Fe atomic clusters (ACs) and satellite Fe-N 4 active sites were fabricated to initiate peroxymonosulfate (PMS) oxidation reaction. The AC-induced charge redistribution of single atoms (SAs) was verified, thus strengthening the interaction between SAs and PMS. In detail, the incorporation of ACs optimized the HSO 5 - oxidation and SO 5 ·− desorption steps, accelerating the reaction progress. As a result, the Vis/TiFeAS/PMS system rapidly eliminated 90.81% of 45 mg/L tetracycline (TC) in 10 min. The reaction process characterization suggested that PMS as an electron donor would transfer electron to Fe species in TiFeAS, generating 1 O 2 . Subsequently, the h VB + can induce the generation of electron-deficient Fe species, promoting the reaction circulation. This work provides a strategy to construct catalysts with multiple atom assembly–enabled composite active sites for high-efficiency PMS-based advanced oxidation processes (AOPs).

Mechanism of Particle-Mediated Inhibition of Demetalation for Single-Atom Catalytic Sites in Acidic Electrochemical Environments

“…At a particle size of 0.7 nm (equivalent to 19 Pt atoms), the farthest interaction distance observed was 0.8 nm, while at a larger particle size of 0.9 nm (27 Pt atoms), the distance increased to 1.5 nm (Figure S9). This long-range interaction has been proposed by several research groups. − …”

Deep Oxidation of Chlorinated VOCs by Efficient Catalytic Peroxide Activation over Nanoconfined Co@NCNT Catalysts

“…Raman spectrum showed that the ratio of I D / I G was determined as 1.01 for Co@NCNT (Figure h), whereas it increased to 1.04 and 1.07 for g-C 3 N 4 and Co@NCNS, respectively (Figure S10). This demonstrated that Co@NCNT exhibited more sp 2 sites and a higher graphitization degree than g-C 3 N 4 and Co@NCNS . Additionally, the EPR signal of Co@NCNT was obviously strengthened (Figure i), indicating its higher concentration of unpaired electrons .…”

“…This demonstrated that Co@NCNT exhibited more sp 2 sites and a higher graphitization degree than g-C 3 N 4 and Co@ NCNS. 34 Additionally, the EPR signal of Co@NCNT was obviously strengthened (Figure 2i), indicating its higher concentration of unpaired electrons. 35 The above physicochemical properties may confer greater electrical conductivity and adsorption capacity of Co@NCNT for chlorobenzene molecules through π−π interactions.…”

Integrated Design of a Dual-Mode Colorimetric Sensor Driven by Enzyme-like Activity Regulation Strategy for Ultratrace and Portable Detection of Hg2+

“…Generally, electron transfer drives the catalytic reaction process, accompanied by the generation of reactive oxygen species (ROS) . Electron transfer exists in the conversion process between different valence states of elements, especially in metal elements as active centers. − The existence of the electron transfer process was verified by a cytochrome C (Cyt C, a common electron transporter) oxidization experiment. Generally, the UV–vis spectrum of Cyt C at a reduced state alone has two absorption peaks at 520 and 550 nm, and a new peak at 530 nm was able to appear once Cyt C was oxidized.…”