ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yachao Wang,Lingfang Liu,Yaxiong Wei,Xinsheng Xu,Guofeng Zhao,Rui Zhong,Cong Fu
Photocatalytic H2O2 production stands as a promising sustainable technology for chemical synthesis. However, rapid charge recombination and limited oxygen adsorption by photocatalysts often limit its efficiency. Herein, we demonstrate that the synergy of Ag and interfacial oxygen vacancies on TiO2 could overcome these challenges. The optimized Ag/TiO2-50 photocatalyst achieved an impressive H2O2 production rate of 12.9 mmol h–1 g–1 and maintained a steady-state concentration of 12.8 mM, significantly outperforming most TiO2-based photocatalysts documented in the literature. Detailed mechanistic studies, aided by TAS, in situ X-ray photoelectron spectroscopy (XPS), and in situ electron paramagnetic resonance (EPR) techniques, indicate that the oxygen vacancies at the Ag–TiO2 interface act as an interfacial hole trap, inducing a directional hole transfer. This, coupled with Ag acting as an electron acceptor, synergistically boosts the electron–hole separation. Additionally, the increased amount of oxygen vacancies at the Ag–TiO2 interface of Ag/TiO2-50 leads to enhanced O2 adsorption, thus contributing to its superior catalytic performance. This study provides valuable insights into interfacial traps in the charge transfer process and highlights the potential of interface regulation for achieving efficient photocatalytic conversion.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
PubMed
高影响因子
PLoS One
·
2018
·Vol. 13
·期 4
·e0192324
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IF 2.766
Hai-qian Zhao,Zhong-hua Wang,Xing-cun Gao,Cheng-hao Liu,Han-bing Qi
H 2 O 2 was adopted to oxidize NO in simulated flue gas at 100–500°C. The effects of the H 2 O 2 evaporation conditions, gas temperature, initial NO concentration, H 2 O 2 concentration, and H 2 O 2 :NO molar ratio on the oxidation efficiency of NO were investigated. The reason for the narrow NO oxidation temperature range near 500°C was determined. The NO oxidation products were analyzed. The removal of NO x using NaOH solution at a moderate oxidation ratio was studied. It was proven that rapid evaporation of the H 2 O 2 solution was critical to increase the NO oxidation efficiency and broaden the oxidation temperature range. the NO oxidation efficiency was above 50% at 300–500°C by contacting the outlet of the syringe needle and the stainless-steel gas pipe together to spread H 2 O 2 solution into a thin film on the surface of the stainless-steel gas pipe, which greatly accelerated the evaporation of H 2 O 2 . The NO oxidation efficiency and the NO oxidation rate increased with increasing initial NO concentration. This method was more effective for the oxidation of NO at high concentrations. H 2 O 2 solution with a concentration higher than 15% was more efficient in oxidizing NO. High temperatures decreased the influence of the H 2 O 2 concentration on the NO oxidation efficiency. The oxidation efficiency of NO increased with an increase in the H 2 O 2 :NO molar ratio, but the ratio of H 2 O 2 to oxidized NO decreased. Over 80% of the NO oxidation product was NO 2 , which indicated that the oxidation ratio of NO did not need to be very high. An 86.7% NO removal efficiency was obtained at an oxidation ratio of only 53.8% when combined with alkali absorption.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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IF 5.8
Yong Tang,Jianhao Qiu,Dingliang Dai,Guanglu Xia,Yixin Li,Biyao Fang,Jianfeng Yao
Sluggish charge transfer dynamics are still the key issue limiting the development of photocatalysis. In this study, CdS/ZnIn 2 S 4 /MIL-53-NH 2 ternary hierarchical heterostructures were constructed via a building block approach, where ZnIn 2 S 4 lamellae first grow on MIL-53-NH 2 followed by CdS nanoparticle deposition. The favorable interfacial compatibility and ternary heterostructures contribute to rapid and multistep spatial charge transfer, which suppresses charge recombination. Therefore, ultrahigh H 2 O 2 production of 1792 μmol·L −1 was obtained over CdS/Znln 2 S 4 /MIL-53-NH 2 composites with visible light, pure water and ambient air, which is not only higher than that of each monomer and binary heterostructure but also better than those of most reported references. Notably, the apparent quantum yield reached 4.5 % at 400 nm, and the solar-to-H 2 O 2 conversion efficiency was 0.081 % in pure water and ambient air. Additionally, H 2 O 2 generation over CdS/Znln 2 S 4 /MIL-53-NH 2 composites involves two-electron O 2 reduction with ·O 2 - as an intermediate. This work may encourage heterostructure design for efficient photocatalytic H 2 O 2 production.
研究领域:
材料科学
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光催化
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纳米技术
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化学工程
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Lele Yang,Hong Chen,Yuntao Xu,Rong Qian,Qiao Chen,Yuanxing Fang
The efficiency of hydrogen peroxide evolution reaction (H 2 O 2 ER) by photoanodic water oxidation is normally limited by low yield and poor selectivity. In this work, the surfaces of Mo doped BiVO 4 are modified by Co 2+ and PO 4 3- ions (CPMB), which has been used as the photoanode with improved H 2 O 2 yield and selectivity. The optimal evolution rate of the CPMB is ca. 0.23 µmol·min −1 ·cm −2 , corresponding to 2.5 times to the pristine BiVO 4 photoanode, and the faradaic efficiency of CPMB photoanode for H 2 O 2 ER is ca. 26%. In this study, the mechanism for the improved H 2 O 2 evolution performance of CPMB has been investigated, indicating that PO 4 3- ions mainly promote the formation of the •OH by dissociation of H 2 O, while Co 2+ ions accelerate the conversion of the •OH for the subsequent H 2 O 2 evolution. This study offers the strategy for designing an efficient photoelectrochemical system with optimized solar conversion efficiency for H 2 O 2 production.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
MICROCHIMICA ACTA
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2022
·Vol. 190
·期 1
·1-12
·
IF 6.408
Yan Zhengquan,Zheng Xiaoyu,Meng Guoqing,Tang Yulian,Zhou Xuemei,Hao Junkai,Feng Jing,Lin Naibo,Hu Lei
A portable sensor for visual monitoring of Fe 2+ and H 2 O 2 , two-dimensional Co 3 O 4 modified by nano-IrO 2 (IrO 2 @2D Co 3 O 4 ) was prepared in this work, for the first time, with the help of microwave radiation at 140 °C, which was further stabilized onto common test strips. The present IrO 2 @2D Co 3 O 4 possessed superior dual-function enzyme-like activity with low toxicity and excellent biocompatibility. Especially, trace Fe 2+ and H 2 O 2 could exclusively alter their enzyme-like catalytic activity with discriminating hyperchromic or hypochromic effect, i.e., from blue to colorless or to dark blue for both IrO 2 @2D Co 3 O 4 dispersion and its functionalized test strips. The linear regression equations were A 652 = 0.5940 − 0.00041 c Fe 2+ (10 −8 M, R 2 = 0.9927) for Fe 2+ and ∆A 652 = 0.0023 c H2O2 + 0.00025 (10 −7 M, R 2 = 0.9982) for H 2 O 2 , respectively. When applied to visual monitoring of aqueous Fe 2+ and intercellular H 2 O 2 , the recoveries were 101.2 ~ 102.5% and 95.8 ~ 103.7% with detection limits of 1.25 × 10 −8 mol/L and 1.02 × 10 −7 mol/L, respectively, far below the permitted values in drinking water set by the World Health Organization. The mechanisms for the enhancing enzyme-mimetic activity of IrO 2 @2D Co 3 O 4 and its selective responses to Fe 2+ and H 2 O 2 were investigated in detail. Graphical Abstract
研究领域:
分析化学
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生物医学工程
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环境科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Shuang Liang,Changhua Wang,Qi Wu,Rui Wang,Yingying Li,Jinglun Du,Xintong Zhang
Solution plasma catalysis has emerged as a promising strategy for the sustainable and rapid production of hydrogen peroxide (H 2 O 2 ) from water and oxygen by clean electricity. However, the uncontrollable electron loss and inefficient utilization of reactive species in solution plasma significantly limit the plasma-to-H 2 O 2 (PTH) conversion efficiency. This lack of control over the plasma environment makes it challenging to design catalysts capable of selectively channeling reactive species toward H 2 O 2 production. Here, we develop modified C 3 N 4 with different functional groups to improve PTH conversion efficiency. The aldehyde-modified C 3 N 4 achieves an unprecedented H 2 O 2 production rate of 4.4 ± 0.1 mM h −1 and a remarkable PTH conversion efficiency of 1.3 %, which is 16 times higher than that of the plasma system without a catalyst. We clarified by density functional calculations and spectroscopic measurements that the improved H 2 O 2 yields and efficiency are due to the modification of the electron-withdrawing groups to promote the generation of 1 O 2 intermediates. This work confirms the critical importance of rational catalyst design to improve PTH conversion efficiency, paving the way for sustainable and rapid solution-based chemical synthesis.
研究领域:
等离子体催化
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材料化学
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可持续能源
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绿色化学
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DOI
高影响因子
ENVIRONMENT INTERNATIONAL
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2019
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IF 7.943
Chao Shan,Yan Liu,Yuhao Huang,Bingcai Pan
Heterogeneous catalysis is a promising approach to achieve efficient As(III) oxidation by H 2 O 2 at circumneutral pH. However, radical-attack pathways dominated catalytic As(III) oxidation over most metal oxides is undesirably associated with low utilization of H 2 O 2 induced by rapid self-quenching of radicals. In this study, we developed a non-radical catalytic route to improve H 2 O 2 utilization efficiency for catalytic As(III) oxidation based on nanoceria. The performance and mechanism of As(III) oxidation by H 2 O 2 was investigated by employing four types of nanoceria with different crystallite sizes (9.1–80.6 nm). At the H 2 O 2 /As(III) molar ratio of 2.0, nanoceria exhibited crystallite size-dependent catalytic activity for oxidation of As(III) over a wide pH range (5–9). Based on comprehensive study including scavenging, enzymatic, and pretreatment experiments and miscellaneous spectroscopy techniques, the catalytic As(III) oxidation over nanoceria was proved to be mainly mediated by the non-radical Ce-hydroperoxo surface complexes, whilst the surface hydroperoxyl radical served as a minor oxidant. In contrast, the roles of dissolved oxygen, homogeneous H 2 O 2 , and OH radical were all negligible. No obvious interconversion of Ce(III)/Ce(IV) was observed by XPS for the catalytic process. Such non-radical pathway enabled a stoichiometric reaction with high H 2 O 2 utilization efficiency (90.5%–122%). Moreover, nanoceria could be recycled for five consecutive runs without desorption/regeneration treatment. This study sheds new light on the development of nanoceria-based catalytic processes for efficient oxidation of As(III).
研究领域:
环境化学
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催化
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水处理
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材料科学
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
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IF 6.4
Xiaoying Bo,Caijie Yang,Bolun Li,Yikang Fan,Jiaoyan Li,Hengming Huang,Jiahui Kou,Chunhua Lu
The photocatalytic O2 reduction to produce H2O2 offers significant environmental benefits. However, its efficiency is hindered by rapid charge recombination and sluggish catalytic kinetics in the catalyst. Traditional elemental doping has been employed to mitigate these issues, but its efficacy is limited as heteroatoms within the bulk often trap charge carriers. To address these challenges, we propose a gradient doping strategy. Unlike uniform doping, gradient doping introduces additional active sites on the catalyst surface. Our engineered gradient Mn-doped CdS photocatalyst demonstrated a remarkable H2O2 generation rate of 1874 μmol g−1 h−1, with an apparent quantum efficiency of 65.2% at 475 nm. The gradient distribution of Mn creates reverse quantum wells within the CdS matrix, which significantly enhances charge extraction from the bulk to the surface. The surface enrichment of Mn not only facilitates the adsorption and activation of O2 but also promotes the formation of the crucial *OOH intermediate, thereby accelerating H2O2 production.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
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2021
·
IF 6.986
Yi Chen,Xiaowen Jiang,Junnan Wang,Zhengxiu Wu,Yuchen Wu,Zhonghua Ni,Hong Yi,Rongsheng Lu
The clinical challenge of high-accuracy blood glucose detection schemes is to overcome the detection error caused by the background interferences in different individuals. H2O2 as the specific product of glucose oxidation can be involved in the Fe2+/Fe3+ conversion and detected by the time-domain nuclear magnetic resonance (TD-NMR) method sensitively. But, in clinical applications, the oxidation of Fe2+ is susceptible to the complex sample substrates. In this work, we sorted out two kinds of possible interference mechanisms of Fe2+ oxidation in the NMR blood glucose detection method and proposed a feasible scheme that uses sorbitol to weaken the adverse effects of interference. We found that sorbitol-mediated Fe2+ can greatly enhance the sensitivity of the T2 value to H2O2. The chain reaction caused by sorbitol can significantly amplify the efficiency of Fe2+ oxidation at the same concentration of H2O2. Thereby, we can achieve the higher dilution multiple of serum samples to reduce the amount of interfering substances involved in the Fe2+/Fe3+ conversion. We justified the accuracy and availability of our method by successfully detecting and confirming the correlation between the T2 decrease and glucose concentration of the serum samples collected from 16 subjects. The sorbitol–Fe2+ glucose detection method with high sensitivity can be further combined with miniature NMR analyzers to satisfy the calibration requirements of glucose monitoring in diabetic patients instead of frequent medical visits.
研究领域:
医学诊断
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生物化学
·
临床医学
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DOI
PubMed
高影响因子
Frontiers in Environmental Science
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2021
·
IF 4.581
You Wen-Dan,Ye Pu,Yang Bin,Luo Xin,Fang Jie,Mai Zi-Tian,Sun Jian-Liang
Benzodiazepines are one group of psychoactive drugs widely detected in water environments, and their persistence during conventional wastewater treatment has raised great concerns. Here we investigated the degradation of 17 benzodiazepines in water by UV/H2O2 treatment. The results showed that the UV/H2O2 treatment significantly increased the degradation of 17 benzodiazepines in phosphate buffer solutions at pH 7.0. This can be attributed to the high reactivity of hydroxyl radicals (·OH) towards benzodiazepines with second-order rate constants of 3.48 × 109 M−1 s−1–2.44 × 1010 M−1 s−1. The degradation of alprazolam, a typical benzodiazepine, during the UV/H2O2 treatment was increased with the increasing H2O2 dosage. The solution pH influenced the alprazolam degradation significantly, with the highest degradation at pH 7.0. Water matrix, such as anions (Cl−, HCO3−, NO3−) and humic acid, decreased the degradation of alprazolam by UV/H2O2 treatment. Based on the degradation products identified using quadrupole time-of-flight mass spectrometer, the degradation mechanisms of alprazolam by UV/H2O2 treatment were proposed, and hydroxylation induced by ·OH was the main reaction pathway. The degradation of 17 benzodiazepines by UV/H2O2 treatment in wastewater treatment plant effluent and river water was lower than that in phosphate buffer solutions. The results showed that the benzodiazepine psychoactive drugs in natural water can be effectively removed by the UV/H2O2 treatment.
研究领域:
环境科学
·
药理学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Muhua Chen,Yiping Liu,Ju Liu,Zilin Kan,Chenhui Sun,Yuqing Wang,Bo Fu,Xinbao Zhu
Recently, photocatalytic production of H 2 O 2 by semiconductors emerges as a green and potential method for green and sustainable H 2 O 2 synthesis. In this work, a g-C 3 N 4 /CAU-17 composite with heterojunction structure was fabricated. There is a tight interface contact between g-C 3 N 4 and CAU-17. And the g-C 3 N 4 nanosheets was uniformly wrapped on CAU-17 surface. In the hybrid catalyst, CAU-17 provides a high surface area for g-C 3 N 4 dispersion and the integration of g-C 3 N 4 boosts the visible light response. Results showed that the H 2 O 2 yield is 419.0 μmol . L −1. h −1 over g-C 3 N 4 /CAU-17 sample, which is 1.59 and 7.83 fold enhancements to bare g-C 3 N 4 and CAU-17 counterparts. This work sheds light on the design of CAU-17-based composite photocatalysts and provides insights into H 2 O 2 synthesis.
研究领域:
材料科学
·
化学工程
·
环境科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
You Wu,Yi Yang,Miaoli Gu,Chuanbiao Bie,Haiyan Tan,Bei Cheng,Jingsan Xu
Solar photocatalysis is a promising, green, and sustainable technique for the synthesis of H 2 O 2 . In this study, low-dimensional ZnO/ZnIn 2 S 4 S-scheme heterojunction photocatalysts are fabricated using electrostatic spinning and chemical bath deposition methods for the efficient photocatalytic production of H 2 O 2 . ZnO nanofibers loaded with 20 wt% ZnIn 2 S 4 exhibit a superior H 2 O 2 production rate of 928 μmol g −1 h −1 , which is more than four times higher than that seen in pristine hexagonal phase ZnO and ZnIn 2 S 4 . First-principles calculations and in-situ X-ray photoelectron spectroscopy reveal the charge separation and transfer mechanisms in the S-scheme heterojunction. The construction of the S-scheme heterojunction facilitates the spatial separation of charge carriers, and electrons and holes with higher redox abilities are retained. Photoelectrochemical and photoluminescence tests further show that the formation of an S-scheme heterojunction is beneficial for the separation of photoinduced charge carriers. Electrochemical tests and electron paramagnetic resonance measurements indicate that H 2 O 2 production is primarily via a two-step single-electron O 2 reduction path. This study provides a new approach for the construction of S-scheme heterojunction materials that can efficiently produce H 2 O 2 under solar irradiation.
研究领域:
材料科学
·
环境科学
·
光催化技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）