Building Feedback-Regulation System Through Atomic Design for Highly Active SO2 Sensing

doi:10.1007/s40820-024-01350-3

Abstract

Abstract:

Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction. Herein, we present an ingenious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO₂ sensing. We found that the single Pt sites on the MoS₂ surface can induce easier volatilization of adjacent S species to activate the whole inert S plane. Reversely, the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms, thus creating a combined system involving S vacancy-assisted single Pt sites (Pt-Vs) to synergistically improve the adsorption ability of SO₂ gas molecules. Furthermore, in situ Raman, ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS₂ supports in SO₂ gas atmosphere. Equipped with wireless-sensing modules, the final Pt₁-MoS₂-def sensors array can further realize real-time monitoring of SO₂ levels and cloud-data storage for plant growth. Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.

Key words: Feedback-regulation system, Atomic interface, SO₂ sensor, Single-atom sensing mechanism, Intelligent-sensing array

Xin Jia, Panzhe Qiao, Xiaowu Wang, Muyu Yan, Yang Chen, Bao-Li An, Pengfei Hu, Bo Lu, Jing Xu, Zhenggang Xue, Jiaqiang Xu. Building Feedback-Regulation System Through Atomic Design for Highly Active SO₂ Sensing[J]. Nano-Micro Letters, 2024, 16(1): 136-.

Xin Jia, Panzhe Qiao, Xiaowu Wang, Muyu Yan, Yang Chen, Bao-Li An, Pengfei Hu, Bo Lu, Jing Xu, Zhenggang Xue, Jiaqiang Xu. [J]. Nano-Micro Letters, 2024, 16(1): 136-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01350-3

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/136

Figures/Tables 7

Fig. 1 The schematic of the feedback-regulation system in the Pt₁-MoS₂-def

Fig. 2 Characterization of Pt₁-MoS₂ and Pt₁-MoS₂-def. a HAADF-STEM image of Pt₁-MoS₂-def. b The intensity profiles obtained in regions X-Y in (a). c, d The atom-overlapping Gaussian-function fitting images of selective area scan (measured from white frame of (a). e, f HAADF-STEM image of Pt₁-MoS₂-def and its simulated image. g Pt L-edge XANES spectra. h FT-EXAFS spectra and i corresponding fitting curve of Pt L₃ edge. j Wavelet transform patterns of Pt foil, PtS₂, Pt₁-MoS₂ and Pt₁-MoS₂-def

Fig. 3 Structural characterizations of Pt₁-MoS₂-def and reference materials. a The diffusion path of Pt atoms on MoS₂-def surface and diagram of S vacancy formation energy. b Electron-paramagnetic resonance images of MoS₂, MoS₂-def, Pt₁-MoS₂ and Pt₁-MoS₂-def. c Mo 3d XPS of MoS_2, Pt₁-MoS₂ and Pt₁-MoS₂-def. d S 2p XPS of MoS_2, Pt₁-MoS₂ and Pt₁-MoS₂-def. e Pt 4f XPS of Pt₁-MoS₂ and Pt₁-MoS₂-def. f The planar-averaged electron density difference ∆ρ(z) of Pt₁-MoS₂ and Pt₁-MoS₂-def

Fig. 4 Gas-sensing performance of MoS₂, Pt₁-MoS₂ and Pt₁-MoS₂-def. a, b Time-related dynamic responses in the concentration range of 0.5-5 and 20-40 ppm. c The responses of MoS₂, Pt₁-MoS₂ and Pt₁-MoS₂-def in different SO₂ concentrations. d RT operation state-of-the-art SO₂ chemiresistors for response. e The selectivity of MoS₂, Pt₁-MoS₂ and Pt₁-MoS₂-def in different gases. f Adsorption and desorption rate constant K_ads and K_des values. g stability tests using sensors upon 8 cyclic exposures to 25 ppm SO₂. (All the sensing tests were conducted at RT in (30%RH) condition)

Fig. 5 The experimental investigation of the mechanism for the gas-sensing property of Pt₁-MoS₂-def. a The SO₂ adsorption curves, b desorption curves and c SO₂ adsorption rate of MoS₂, Pt₁-MoS₂, Pt NPs-MoS₂ and Pt₁-MoS₂-def. The ex situ XPS spectra of d Pt₁-MoS₂ and e Pt₁-MoS₂-def. f In situ Raman spectra of the Pt₁-MoS₂ and Pt₁-MoS₂-def. g Two different path types of Pt₁-MoS₂ and Pt₁-MoS₂-def with SO₂. h In-situ SO₂ adsorption breakthrough curves of MoS₂, Pt₁-MoS₂ and Pt₁-MoS₂-def at 25 °C

Fig. 6 The theoretical investigation of the mechanism for the gas-sensing property of Pt₁-MoS₂-def. a PDOS for Pt 4d orbital and the d band center of Pt₁-MoS₂ and Pt₁-MoS₂-def. b pCOHP and c ICOHP of terminal Pt-S bonds of Pt₁-MoS₂ and Pt₁-MoS₂-def. d The partial density of states (pDOS) analysis and adsorption energy of SO₂/Pt₁-MoS₂-def, SO₂/Pt₁-MoS₂ and SO₂/MoS₂ models. The electronic transfer between SO₂ and e Pt₁-MoS₂-def and f Pt₁-MoS₂ sample. The yellow and blue lobes represent the accumulation and depletion of charge. g Mechanism for tailoring the level of antibonding-orbital occupancy state to unidirectionally determined the gas-sensing property of SO₂

Fig. 7 Pt₁-MoS₂-def-based SO₂ gas sensors for monitoring the plants growth. a Schematic of real-time detection of SO₂ gas concentration in a greenhouse. b Photo of the device in a simulated greenhouse with plants, with a smartphone and Bluetooth and data transmission. c Corresponding block modules. d Block diagram of the whole system. e Data measured by this device

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