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Journal of Materials Chemistry C · 2022 ·Vol. 10 ·期 9 ·3500-3509 · IF 8.067

Nitrogen-doped biochar nanosheets facilitate charge separation of a Bi/Bi2O3 nanosphere with a Mott–Schottky heterojunction for efficient photocatalytic reforming of biomass

Dongnv Jin,Jiliang Ma,Runcang Sun

Coupling a semimetal with a semiconductor on nitrogen-doped carbon for photocatalytic reforming of biomass-derived feedstocks into high value-added chemicals is of great significance; however, no success has been achieved to date. Here, uniformly dispersed Bi/Bi2O3 nanospheres with a Mott–Schottky heterojunction embedded on the nitrogen-doped biochar nanosheets (Bi/Bi2O3@N-BC) were developed and successfully used in photocatalytic biomass-reforming to lactic acid. A built-in electric field between the interfaces of Bi and Bi2O3 was constructed via the Schottky effect of the Bi/Bi2O3 heterojunction, resulting in the rapid separation/migration of electrons–holes; whereas the N-BC facilitates the adsorption of reactants and the mass transfer of products or by-products. The highest yield of lactic acid reached was 91.21%, and Bi/Bi2O3@N-BC displayed excellent stability, reusability and universality. The experimental results indicated that the contents of photoinduced h+, ˙O2−, ˙OH and 1O2 increased with prolonging the visible-light irradiation time, and trapping tests suggested that ˙O2−, 1O2 and h+ promoted the lactic acid production in turn, whereas ˙OH inhibited the reaction. A 1000-fold scale-up experiment showed that the economically and environmentally viable system has potential for application in the industrial production of lactic acid, and this work also provides an efficient strategy for the development of functional photocatalysts and photocatalytic biorefinery.

研究领域: 材料科学 · 化学工程 · 环境科学 · 催化 · 生物工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Critical roles of soil composition and pollutant properties on the degradation of PPCPs during ferrous/persulfate processes

Lulu Chen,Xinyuan Zhang,Ruonan Feng,Xiaona Dong,Junhe Lu,Canlan Jiang

Pharmaceuticals and personal care products (PPCPs) are widely used worldwide and cause potential soil pollution. Fe 2+ -activated persulfate (PS) processes (Fe-PAPs) are promising techniques for soil remediation. However, a knowledge gap exists in the mechanistic insights into the dominant factors affecting the degradation of different PPCPs in varied soil types. This study systematically investigated the roles of soil components and pollutant properties in the degradation of three PPCPs (triclosan (TCS), triclocarban (TCC), and naproxen (NPS)) in the nine soils in the Fe 2+ /PS system. The degradation efficiencies of TCS and NPS ranged from 10.92 % to 91.62 % and 46.59 % to 99.81 %, respectively, whereas nearly no degradation was observed for TCC. PPCPs with high water solubility, high energies of the highest occupied molecular orbital (E HOMO ), low p K a values, low energy gap (ΔE), or low vertical ionization potential (VIP) were more favorable for degradation. XPS analysis suggested that aliphatic carbon (Ali–C–C(H)), ether or alcohol carbon (C–O), and aldehyde or ketonic carbon (C O) on SOM significantly inhibited TCS degradation. The results of ROS quenching experiments showed that SO 4 •− and 1 O 2 played major roles in TCS and NPS degradation in the six soils, with the relative contributions ranged from 24.82 % to 99.14 % and 0.15 % to 73.40 %, respectively. The interaction between soil components, active species, and pollutants resulted in the distinct intermediates of TCS and NPS in different soils. Our findings provide in-depth insights into the role of soil composition and pollutant properties on the remediation of PPCP-contaminated soils in Fe-PAPs.

研究领域: 环境科学 · 土壤化学 · 污染物降解 · 药物化学
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APPLIED CATALYSIS A-GENERAL · 2022 · IF 5.723

Dual-functional Mo2C quantum dots enriched N-doped graphitic carbon layers in advanced oxidation processes (AOPs)

Chencheng Dong,Yan Bao,Mingyang Xing,Masakazu Anpo,Jinlong Zhang

Advanced oxidation processes (AOPs) are reckoned effective for removing persistent and recalcitrant pollutants by reactive oxygen species (ROSs), including hydroxyl radicals (•OH), sulfate radicals (SO 4 • - ), and superoxide radicals (•O 2 - ), as well as singlet oxygen ( 1 O 2 ). In this work, the Mo 2 C quantum dots enriched N-doped graphitic carbon layers (Mo 2 C QDs/NGCLs) were constructed via a facile two-step methodology. Interestingly, the Mo 2 C QDs/NGCLs acted as a highly efficient cocatalyst and/or catalyst simultaneously in AOPs, in particular visible-light-driven (VLD) Fenton and VLD PMS activation. In the hydroxyl radical-based AOPs (•OH-AOPs), it exhibited a remarkable removal efficiency for a range of aromatic organic pollutants , including rhodamine B (RhB) (99.9 %), phenol (90 %), benzophenone-3 (BZP) (83 %), methyl orange (MO) (58 %), methyl blue (MB) (89 %), ibuprofen (IBU) (100 %), and carbamazepine (CBZ) (50 %). Sulfate radicals-based AOPs (SR-AOPs) effectively degrade RhB (72 %), MO (83 %), IBU (70 %), and BZP (100 %). Thus, the present findings confirmed the potential of transition metal carbides for AOP applications and established a solid theoretical and technical basis for further research.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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Journal of Cleaner Production · 2023 · IF 11.1

Research on the reaction path of chlorobenzene oxidation by electrochemical-sodium persulfate system

Shicheng Yuan,Hui Hu,Hao Huang,Zhongming Chen,Jiaxin Chen,Mi Zhang,Kunpeng Li,Ting Zhou,Ruibin Lv

Chlorobenzene (CB) is an important organic chemical material that is volatile and difficult to degrade, and has received much attention because of its strong ozone generation potential. An electrochemical-sodium peroxydisulfate (PDS) system was constructed and the oxidation reaction path of chlorobenzene in this system was analyzed. The effects of current density, PDS concentration, initial pH, CB blow-off gas ratio and temperature on the oxidation and mineralization rate of chlorobenzene in the system were investigated respectively. At a current density of 168 A/m 2 , a PDS concentration of 0.5 mol/L, an initial pH of 10, a CB blow-off gas ratio of 20% and a reaction temperature of 60 °C, the CB conversion and mineralization rates were able to reach more than 90%. The results of electron paramagnetic resonance (EPR) experiments using 5,5-dimethyl-1-pyrroline N-oxide (DMPO) and 2,2,6,6-tetramethyl-4-piperidone hydrochloride (TEMP) as spin trapping agents indicate the presence of ⦁OH, · S O 4 − and 1 O 2 in the system. The signal of · O 2 − was also captured after the quenching of ⦁OH, which further indicates the presence of 1 O 2 . And the results of active substance quenching experiments showed that the active species that mainly contributed to the oxidation of chlorobenzene included ⦁OH, · S O 4 − and 1 O 2 , and their contributions to the oxidation of chlorobenzene were 25.0%, 31.7% and 22.2%, respectively. The Liquid Chromatograph Mass Spectrometer (LC-MS) characterization results showed that the formation of chlorophenol and hydroquinone and their ring-opening reactions were the most critical processes in the oxidative decomposition of chlorobenzene, and the reaction pathways for the oxidation of chlorobenzene by ⦁OH, · S O 4 − and 1 O 2 were proposed by these characterization results.

CAS / MDL: 3317-61-1
研究领域: 环境科学 · 化工工程 · 分析化学
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