Lim Dae-Hwan, Maitlo Hubdar Ali, Younis Sherif A, Boukhvalov Danil W, Kim Ki-Hyun, Lee Jechan
Department of Civil and Environmental Engineering, Hanyang University, Seoul 04763, Republic of Korea.
Department of Civil and Environmental Engineering, Hanyang University, Seoul 04763, Republic of Korea; Department of Energy and Environment Engineering, Dawood University of Engineering and Technology, Karachi 74800, Pakistan.
J Colloid Interface Sci. 2025 Sep 3;702(Pt 1):138895. doi: 10.1016/j.jcis.2025.138895.
Platinum and nitrogen co-doped titanium dioxide (Pt/N-TiO, with 1 wt% Pt and an N/Ti molar ratio of 1) has been synthesized. This Pt/N co-doping strategy creates Schottky junctions, reduces the bandgap energy (3.25 to 2.12 eV), and introduces a new energy level (N 2p). The modified catalyst exhibits dual functionality, serving as both a photocatalyst under light irradiation (λ = 365 nm, 32 W) and a light-free catalytic adsorbent against gaseous formaldehyde (FA). The Pt/N-TiO catalysts are immobilized on ceramic bead supports, placed in a tubular reactor system, and tested under controlled operating conditions, including FA concentrations (100-500 ppm), oxygen levels (0-21%), relative humidity (RH; 0-100%), and gas flow rates (100-500 mL min). The Pt/N-TiO achieves a photocatalytic oxidation efficiency of 94.2% (reaction rate of 9.24 μmol mg h and apparent quantum yield of 5.58%) against 200 ppm FA (100% RH). The catalyst's efficiency stems from a synergistic dual mechanism, as evidenced by molecular simulation using density functional theory. First, N doping enhances light absorption and extends the charge carrier lifetime, while the Pt as a co-catalyst promotes charge separation by acting as an electron sink. Second, the catalyst's ability to efficiently trap HO and O molecules also contributes to the efficient mineralization of FA through the facile generation of reactive oxygen species. This dual functionality extends to dark conditions as a catalytic adsorbent, achieving a FA removal efficiency of 78.9% with a CO yield of 57%. In-situ diffuse reflectance infrared Fourier transform spectroscopy analysis confirms this mechanism by identifying the generation of Pt-OH hydroxylation and O radicals from HO vapor and O, respectively. Overall, this research provides a practical guideline for constructing an advanced VOC abatement platform.
已合成了铂和氮共掺杂的二氧化钛(Pt/N-TiO₂,含1 wt%的Pt且N/Ti摩尔比为1)。这种Pt/N共掺杂策略形成了肖特基结,降低了带隙能量(从3.25 eV降至2.12 eV),并引入了一个新的能级(N 2p)。改性后的催化剂具有双重功能,在光照射(λ = 365 nm,32 W)下作为光催化剂,同时作为针对气态甲醛(FA)的无光催化吸附剂。将Pt/N-TiO₂催化剂固定在陶瓷珠载体上,置于管式反应器系统中,并在包括FA浓度(100 - 500 ppm)、氧气水平(0 - 21%)、相对湿度(RH;0 - 100%)和气体流速(100 - 500 mL min⁻¹)等受控操作条件下进行测试。对于200 ppm的FA(100% RH),Pt/N-TiO₂实现了94.2%的光催化氧化效率(反应速率为9.24 μmol mg⁻¹ h⁻¹,表观量子产率为5.58%)。催化剂的效率源于协同双重机制,这由使用密度泛函理论的分子模拟所证实。首先,N掺杂增强了光吸收并延长了电荷载流子寿命,而作为助催化剂的Pt通过充当电子阱促进电荷分离。其次,催化剂有效捕获HO·和O₂分子的能力也通过易于产生活性氧物种而有助于FA的高效矿化。这种双重功能在黑暗条件下作为催化吸附剂也能实现,FA去除效率达到78.9%,CO₂产率为57%。原位漫反射红外傅里叶变换光谱分析通过分别识别来自HO·蒸气和O₂的Pt - OH羟基化和O·自由基的生成来证实这一机制。总体而言,本研究为构建先进的挥发性有机化合物减排平台提供了实用指南。