Molecular Catalysis
·
2023
·
IF 4.6
Wei Tian,Yonggang Dong,Hong Qin,Ziming Luo,Qian Lin,Zheng Chen,Hongyan Pan,Yongyong Shi,Keliang Wang
The direct synthesis of hydrogen peroxide (DSHP) from hydrogen and oxygen is a green synthesis method with a high atomic economy. However, H 2 O 2 selectivity and productivity remain a key challenge, the O O bonds are easily broken with supported Pd catalysts to produce water. Herein, we report the synthesis of bimetallic catalyst PdSn@Pd@HCS by adapting reversed-phase micellar and galvanic replacement reaction. The novel bimetallic yolk-shell structure catalysts exhibit excellent catalytic performance, the selectivity and productivity of H 2 O 2 reaching 98% and 4899 mmol/g Pd· h − 1 , respectively. Theoretical calculations reveal that the presence of Sn inside the bimetallic alloy can enhance the ligand effect and optimize the electronic structure of the surface Pd atoms, weakening the adsorption ability of O 2 molecules and inhibiting the dissociation of O O bonded species, resulting in the enhancement of H 2 O 2 selectivity and productivity. This work provides the groundwork for bimetallic yolk-shell structure catalysts to achieve the efficient synthesis of H 2 O 2 .
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lijun Hu,Zhichao Ding,Fei Yan,Yi-Meng Du,Qianxiang Xiao,Hongqing Wang
The conversion of superoxide radical (·O 2 − ) to hydrogen peroxide (H 2 O 2 ) is critical in the photocatalytic formation of H 2 O 2 via the sequential two-step single-electron oxygen reduction mechanism. Providing a high concentration of ·O 2 − is an effective approach to promoting this process in terms of chemical kinetics. It is, however, extremely challenging to implement this idea in the photocatalytic solution due to the limited lifespan of ·O 2 − . To this end, a concept about local ·O 2 − enrichment catalyst surface was proposed in this study and achieved in an innovative PSI/C 3 N 4 photocatalyst. The results of theoretical calculations and temperature-dependent photocatalytic studies indicate that PSI on the C 3 N 4 surface can serve as a diffusion buffer for ·O 2 − , capturing them through Van der Waals interactions and separating them by energy perturbations. As a result, a local enrichment of ·O 2 − was established on the PSI/C 3 N 4 surface during photocatalysis, strengthening the photocatalytic conversion of ·O 2 − to H 2 O 2 , thus allowing the PSI/C 3 N 4 -4 photocatalyst to produce H 2 O 2 at a rate of approximately 2.4 and 2.65 times greater than pure C 3 N 4 under visible light and LED irradiation, respectively. This study presents a promising strategy for enhancing photocatalytic H 2 O 2 production efficiency by selectively enriching ·O 2 − on the catalyst surface.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 11
·e18192
·
IF 3.7
Guanglu Xia,Jianhao Qiu,Dingliang Dai,Lu Zhang,Yong Tang,Jianfeng Yao
A series of covalent organic frameworks (COFs) with β-ketoenamine linkages named TpTt-COF, TAPT-COF, and TpPa-1 were constructed for photocatalytic H 2 O 2 generation in pure water and ambient air under visible light. Among them, TpTt-COF performed striking H 2 O 2 yield of 2647 μmol L −1 , which is 3.5, 17.5, and 176.5-fold those of TAPT-COF, TpPa-1, and bulk g-C 3 N 4 , respectively, attributing to the electron-deficient trait, short charge diffusion distance, and the narrowest bandgap of TpTt-COF. Additionally, to achieve the facile recovery, TpTt-COF was firmly and evenly anchored on melamine sponges (MS) because plenty of amino groups on the surface of MS could be involved in the β-ketoenamine formation and guide the synthesis of TpTt-COF on MS. The corresponding H 2 O 2 evolution over this photocatalyst monolith is also respectable and can be well repeated at least four times. This work is quite instructive for photocatalyst construction based on covalent organic frameworks and facile photocatalytic applications.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Sun Lina,Sun Liping,Huo Lihua,Zhao Hui
The production of hydrogen peroxide (H 2 O 2 ) through electrochemically reducing O 2 in a two-electron pathway is a potential substitute for the traditional process based on anthraquinone. In this paper, F doping is carried out to prepare N and F co-doped porous carbon embedded Co nanoparticles. The electro-catalytic activity for the electrochemical production of H 2 O 2 is systematically investigated. The composite material demonstrates exceptional electro-catalytic selectivity, reaching approximately 92.5%, and shows an ultra-high rate of producing H 2 O 2 in 4021.4 mmol g -1 h -1 at 0.1 V versus RHE in a 0.5 M H 2 SO 4 electrolyte. It is found that the synergetic effect of Co-Nx and F in the composite material result in its exceptional performance. Adding F atom modulates the Zeta potential of the catalyst and alters the electronic configuration around Co-Nx, creating favorable conditions for the uptake of O 2 and consequently forming OOH*. Additionally, the highly electronegative F atom facilitate desorbing OOH* through electrostatic repulsion, preventing any further degradation. In a homemade electrolyzer containing 80 mg L -1 of Rh B, the H 2 O 2 produced in situ in a 0.5 M H 2 SO 4 electrolyte degrades up to 97.76% of Rh B in just 22.5 min, showcasing its potential for practical wastewater treatment applications.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Chengcheng Qi,Yuhua Luo,Yongping Dong
The study of single atoms in the field of electrochemical sensing is at the early stage. How to boost the catalytic performance of single atoms is still a big challenge. Herein, we prepare Fe-Se dual single-atom sites on N-doped ultrathin carbon carrier (Fe 1 Se 1 /NC) for realizing highly sensitive nonenzymatic detection of H 2 O 2 . Fe 1 Se 1 /NC was synthesized through the pyrolysis strategy, and then was characterized by transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS) mapping, high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), and electrochemical techniques, respectively. The results displayed that Fe and Se both existed in an atomically dispersed status. Compared to the single-atom Se or Fe catalyst (Se 1 /NC or Fe 1 /NC), the Fe 1 Se 1 /NC significantly boosted the electrocatalytic activity for H 2 O 2 reduction. The Fe 1 Se 1 /NC modified electrode could be used to detect H 2 O 2 in a wide linear range of 0.02 mM to 13 mM with a high sensitivity of 1508.6 µA·mM −1 ·cm −2 and a low detection limit of 11.5 µM. Moreover, the sensor was successfully employed for detecting H 2 O 2 in disinfectant and urine samples. This work provides a novel design of dual-atom catalysts for excellent electrochemical sensing applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yi Yang,Jingjing Liu,Miaoli Gu,Bei Cheng,Linxi Wang,Jiaguo Yu
Coupling photocatalytic H 2 O 2 evolution with simultaneous furfuryl alcohol oxidation can avoid the slow water oxidation reaction and fully utilize photogenerated carriers to produce valuable chemicals. Herein, a COF (denoted as BTTA) was synthesized by the Schiff-base condensation and in-situ grown on the surface of TiO 2 nanofibers. The resultant TiO 2 /BTTA composite has a large interface and a short carrier migration distance. Furthermore, the porous and ultrathin BTTA layers endow the composites abundant active sites and excellent light absorption ability. Remarkably, a H 2 O 2 -evolution rate of 740 μmol L −1 h −1 and a furoic alcohol conversion of 96 % are achieved. In-situ irradiated X-ray photoelectron spectroscopy and electron spin resonance confirm the S-scheme carrier transfer mechanism, which spatially separates photogenerated carriers with strong redox power. This work opens a new door to the rational design of S-scheme photocatalysts for economic and green photosynthesis of H 2 O 2 and organic compounds.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Chengcheng Qi,Wei Xiang,Yongping Dong,Wangbing Zhang
The development of new highly active electrocatalysts is one of the key factors to improve the performance of enzyme-free electrochemical sensors . In this paper, Co 3 V 2 O 8 was proposed as a new electrocatalyst for nonenzymatic oxidation of H 2 O 2 . A facile self-templating strategy was adopted for the synthesis of Co 3 V 2 O 8 nanomaterial which was further characterized by transmission electron microscopy (TEM), powder X-ray diffractometry (XRD), fourier translation infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and electrochemical techniques . The results showed that porous Co 3 V 2 O 8 sphere was constructed from interconnected nanoparticle with a three-dimensional porous structure. Such unique structure made the sensor based on Co 3 V 2 O 8 exhibit good electrocatalytic activity toward H 2 O 2 oxidation, and could detect H 2 O 2 with a low detection limit of 0.34 µM, a wide linear range of 2.0 µM to 6.1 mM and a high sensitivity of 541.4 µA mM −1 cm −2 . This work demonstrated an effective new sensing platform for nonenzymatic detection of H 2 O 2 .
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Nanomaterials
·
2023
·Vol. 13
·期 7
·1188
·
IF 5.3
Lina Sun,Liping Sun,Lihua Huo,Hui Zhao
H2O2generation via an electrochemical two-electron oxygen reduction (2e−ORR) is a potential candidate to replace the industrial anthraquinone process. In this study, porous carbon catalysts co-doped by nitrogen and oxygen are successfully synthesized by the pyrolysis and oxidation of a ZIF-67 precursor. The catalyst exhibits a selectivity of ~83.1% for 2e−ORR, with the electron-transferring number approaching 2.33, and generation rate of 2909.79 mmol g−1h−1at 0.36 V (vs. RHE) in KOH solution (0.1 M). The results prove that graphitic N and –COOH functional groups act as the catalytic centers for this reaction, and the two functional groups work together to greatly enhance the performance of 2e−ORR. In addition, the introduction of the –COOH functional group increases the hydrophilicity and the zeta potential of the carbon materials, which also promotes the 2e−ORR. The study provides a new understanding of the production of H2O2by electrocatalytic oxygen reduction with MOF-derived carbon catalysts.Keywords:porous carbon;two-electron reduction of oxygen;hydrogen peroxide;electrocatalyst
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Hao Ding,Gongsong Tong,Jingchun Sun,Jiewei Ouyang,Fangge Zhu,Zhi Zhou,Nan Zhou,Mei’e Zhong
Biochar, as an adsorbent, is widely used for the removal of organic pollutants in water body. Hence, after saturated adsorption, regeneration treatment is required to recover the adsorption performance of biochar. In this study, a biochar (P-GBC) prepared by phosphoric acid activation showed high adsorption capacity for methylene blue (MB) with the maximum adsorption capacity (Q m ) of 599.66 mg/g. Then, regeneration treatments using 4 mM peroxymonosulfate (PMS), 0.2 M hydrogen peroxide (H 2 O 2 ) and their mixture were used to regenerate MB-saturated biochar with regeneration efficiencies of 58.24%, 66.01% and 94.88%, respectively. Combining with degradation and quenching experiments, it is found that synergistic effect of H 2 O 2 desorption and PMS degradation is responsible for the enhancement of regeneration efficiency of P-GBC in H 2 O 2 -PMS system and enables a high mineralization rate of 82.68% for the MB adsorbed on P-GBC. Furthermore, EPR tests indicate that singlet oxygen ( 1 O 2 ) is assigned as the primary activate species for the degradation of MB and XPS analyses confirm that graphite nitrogen and carbonyl on P-GBC are the main active sites for the activation of PMS. Compared with conventional regenerants, H 2 O 2 -PMS system has the advantages of low dosage, high mineralization efficiency, and easy accessibility, and is also effective, sustainable and environmentally friendly for the regeneration of organic pollutants-saturated biochar.
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FlatChem
·
2023
·
IF 6.2
Anchao Zhou,Tianqi Yu,Xincheng Liang,Shibin Yin
Hydrogen peroxide (H 2 O 2 ) is required to reduce the residual potassium permanganate (KMnO 4 ) in the traditional Hummers method for preparing graphene oxide (GO), which is dangerous and uncontrollable. In this work, spontaneous-reduction of high-valence Mn ions is induced by simply adjusting the reaction temperature/time and the dosage of concentrated sulfuric acid (H 2 SO 4 ) to prepare high quality GO without H 2 O 2 , avoiding the high risk of the dramatically exothermic reduction reaction caused by the quenching reaction of adding H 2 O 2 . Notably, the C/O ratio of GO prepared by this H 2 O 2 -free method is 1.986, which is less than commercial GO. Herein, this work provides a novel and efficient strategy for the safe and environmentally-friendly preparation of GO with high quality.
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ULTRASONICS SONOCHEMISTRY
·
2022
·
IF 9.336
Xia Ma,Lin Dong,Yan He,Shiwen Chen
Yeast β-glucan (YG) possess an extensive range of biological activities, such as the inhibition of oxidation, but the poor water solubility of macromolecular YG limits its application. In this study, through the combined degradation of ultrasonic waves and H 2 O 2 , and the optimization of the main process parameters for solubilizing YG by response surface methodology (RSM), a new product of YG UH was generated. The molecular weight, structural characteristics and degradation kinetics before and after solubilization were evaluated. The results showed that the optimal solubilization conditions were reaction time: 4 h, ultrasonic power: 3 W/mL, H 2 O 2 concentration: 24 %. Under these conditions, ultrasound-assisted H 2 O 2 increased the solubility (from 13.60 % to 70.00 %) and reduced molecular weight (from 6.73 × 10 6 Da to 1.22 × 10 6 Da). Fourier transform infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), Congo red (CR), scanning electron microscopy (SEM) revealed that ultrasound-assisted H 2 O 2 increased the conformation's flexibility greatly, without changing the main structure of YG. More importantly, solubilization of YG improved free radical scavenging activity with YG UH exhibiting the highest levels of DPPH and ABTS + free radical scavenging activity. These results revealed that ultrasound-assisted H 2 O 2 degradation could be a suitable way to increase the solubility of YG for producing value-added YG.
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高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 7
·2101-2107
·
IF 5
Jianhao Qiu,Lu Zhang,Guanglu Xia,Dingliang Dai,Yong Tang,Jianfeng Yao
Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) were prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water. The H2O2 yields using ZnIn2S4/UiO-66-NH2, ZnIn2S4/UiO-66-(OH)2 and ZnIn2S4/UiO-66-OH are 799, 733 and 165 μmol L−1, respectively, which are 9.5, 8.7 and 2.0 times that of ZnIn2S4/UiO-66. The high performance of ZnIn2S4/UiO-66-NH2 and ZnIn2S4/UiO-66-(OH)2 is ascribed to the benign visible-light response and Z-scheme heterostructures, and the H2O2 evolution abides by indirect O2 reduction with ˙O2− as an intermediate species. Additionally, H2O2 yields using ZnIn2S4/UiO-66-NH2 on tap water and Xuanwu Lake (Nanjing, China) water can be comparable to that on the above-deionized water. This study sheds light on the great promise of functionalized MOFs and their applications on green (photo)catalytic energy conversion.
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