MOLECULES
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2024
·Vol. 29
·期 2
·493
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IF 4.2
Ligang Ma,Chao Lin,Wenjun Jiang,Shun Yan,Huilin Jiang,Xiang Song,Xiaoqian Ai,Xiaoxiao Cao,Yihuan Ding
Selective supported catalysts have emerged as a promising approach to enhance carrier separation, particularly in the realm of photocatalytic hydrogen production. Herein, a pioneering exploration involves the loading of PdS and Pt catalyst onto g-C3N4nanosheets to construct g-C3N4@PdS@Pt nanocomposites. The photocatalytic activity of nanocomposites was evaluated under visible light and full spectrum irradiation. The results show that g-C3N4@PdS@Pt nanocomposites exhibit excellent properties. Under visible light irradiation, these nanocomposites exhibit a remarkable production rate of 1289 μmol·g−1·h−1, marking a staggering 60-fold increase compared to g-C3N4@Pt (20.9 μmol·g−1·h−1). Furthermore, when subjected to full spectrum irradiation, the hydrogen production efficiency of g-C3N4@PdS@Pt-3 nanocomposites reaches an impressive 11,438 μmol·g−1·h−1, representing an eightfold enhancement compared to g-C3N4@Pt (1452 μmol·g−1·h−1) under identical conditions. Detailed investigations into the microstructure and optical properties of g-C3N4@PdS catalysts were conducted, shedding light on the mechanisms governing photocatalytic hydrogen production. This study offers valuable insights into the potential of these nanocomposites and their pivotal role in advancing photocatalysis.
研究领域:
材料科学
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能源科学
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DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 67
·54769-54776
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IF 3.84
Chunxiao Lu,Yang Chen,Yun Li,Chunhong Ma,Hongbo Zhang,Yuwei Guo,Jun Wang
A highly effective and stable up-conversion luminescence agent, Er3+:Y3Al5O12, was synthesized by sol–gel and calcination methods. Then, as a novel visible-light photocatalyst, Er3+:Y3Al5O12, Pt and PdS (as dual co-catalysts) decorated ZnS nano-sized composites, Er3+:Y3Al5O12/Pt–PdS/ZnS, were fabricated by deposition–precipitation and ultrasonic dispersion methods. All prepared samples were characterized by X-ray diffractometry (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDX). UV-vis absorption and PL spectra of Er3+:Y3Al5O12 were also determined. The visible-light photocatalytic H2 production activity of the prepared Er3+:Y3Al5O12/Pt–PdS/ZnS was evaluated by using Na2S and Na2SO3 as sacrificial reagents in an aqueous solution under 300 W irradiation from a xenon lamp. In addition, some influential factors such as Er3+:Y3Al5O12 and ZnS mass ratio, catalyst amount, irradiation time and irradiation intensity on visible-light photocatalytic H2 production of Er3+:Y3Al5O12/Pt–PdS/ZnS were investigated in detail. It was found that Er3+:Y3Al5O12 can effectively improve the visible-light photocatalytic activity of ZnS. Particularly, Er3+:Y3Al5O12/Pt–PdS/ZnS with 0.13 wt% PdS and 0.3 wt% Pt and a 0.30 : 1.00 mass ratio shows the highest photocatalytic H2 production activity in the sulfide/sulfite (0.2 mol L−1 Na2S and 0.3 mol L−1 Na2SO3) aqueous solution as sacrificial reagents.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Wenting Li,Hanjie Zhang,Sijie Huang,Jingyi Xu,Liping Liu,Junshan Li,Jianfang Jing,Yongfa Zhu
The efficient activation of peroxydisulfate (PDS) for wastewater treatment remains a great challenge. Photocatalysis, which generates highly-reactive electrons and holes, shows great potential in activating PDS for effective degradation and deep mineralization. Herein, an electron-enriched PDI-SiO 2 photocatalyst was synthesized by covalently linking 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) onto silicon dioxide (SiO 2 ) to form π-π stacked supramolecular PDI layers for efficient PDS activation. The highly dispersed PDI generates electron-enriched PDI· - under visible light, promoting the rapid activation of PDS for bisphenol A (BPA) degradation. The PDI-SiO 2 activated PDS system realized a high BPA degradation rate of 0.100 min −1 and a remarkable mineralization rate of 81%. Moreover, the charge separation efficiency is significantly improved since the electrons of PDI· - are captured by PDS, boosting oxidative degradation and improving the mineralization efficiency. This work developed a novel PDS activation strategy by constructing electron-enriched photocatalyst, and revealed the mechanism of photocatalytic activation and deep mineralization.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Yi Li,Shan Yu,Dmitry E. Doronkin,Shiqian Wei,Meng Dan,Fan Wu,Liqun Ye,Jan-Dierk Grunwaldt,Ying Zhou
As an important byproduct during natural gas exploitation, green utilization of hydrogen sulfide (H 2 S) by photocatalysis has offered us the possibility for production of clean hydrogen (H 2 ) from H 2 S with low energy consumption. In this work, we have successfully introduced well-dispersed palladium sulfide (PdS) which is preferably loaded on In 2 S 3 of MnS/In 2 S 3 composite for improved photocatalytic hydrogen evolution from H 2 S aqueous solution. In contrast to binary MnS/In 2 S 3 , ternary MnS/In 2 S 3 /PdS has exhibited a remarkable and stable hydrogen production rate of 22.7 mmol g −1 h −1 with an apparent quantum yield of 34% at around 395 nm. A comprehensive structure characterization of the ternary composite including scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS) in combination with theoretical calculations confirm the good dispersion of PdS in the composite. Moreover, we discovered that PdS preferably interact with In 2 S 3 rather than MnS in the composite through Pd-S-In bond on the interface of the two. Photoluminescence (PL) spectra, surface photovoltage (SPV) spectra together with transient photocurrent and electrochemical impedance spectra (EIS) demonstrate the advantage of PdS for promoting the charge separation. This work sheds light on the positive effect on the enhanced activity of the corresponding system resulting from the preferable anchoring of highly dispersed PdS on In 2 S 3 in the composite by chemical Pd-S-In bond. Not only the high dispersion but also the preferable anchoring of the co-catalyst in the composite could hence inspire people for more rational designs of ternary composite in future.
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
CHINESE JOURNAL OF CATALYSIS
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2023
·
IF 16.5
Xiao-Juan Li,Ming-Yu Qi,Jing-Yu Li,Chang-Long Tan,Zi-Rong Tang,Yi-Jun Xu
The simultaneous utilization of photogenerated electrons and holes in one cooperative photoredox system for the dehydrocoupling of thiols into value-added disulfides and clean hydrogen (H 2 ) fuel meets the development criteria of green chemistry. Herein, we report the synthesis and application of cocatalyst PdS decorated ZnIn 2 S 4 (PdS-ZIS) composites for photocatalytic coupling of thiols into disulfides and H 2 evolution under visible light irradiation. The superior photocatalytic performance over PdS-ZIS composites compared with blank ZIS is attributed to the function of PdS as oxidation cocatalyst, which dramatically promotes the separation and transfer of photogenerated charge carriers due to its excellent hole trapping ability. In-situ Fourier transform infrared spectra reveal the dynamic variation of reactants on the catalyst surface. Electron paramagnetic resonance technology confirms that sulfur-centered radicals are the key reaction intermediates in this coupling process. Moreover, the application of PdS-ZIS composites to the dehydrocoupling of various thiols with different substituent groups into the corresponding S–S coupling products has been demonstrated to be practicable. This work is expected to offer insights into the rational design of cocatalyst-decorated semiconductor photocatalysts with efficient utilization of photogenerated electrons and holes for the co-production of high-value chemicals and clean H 2 energy in a cooperative photoredox catalysis process.
研究领域:
化学
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材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Yingzi Lin,Mengshi Wang,Junjie Chen,Siwen Li,Yuanyuan Zhang,Liangliang Wei,Ningning Sun,Chengyu Liu,Junjie Zhao
Based on the deficiency of the Fe 2+ catalyzed persulfate (PDS) process, ultraviolet (UV) synergistic Fe 2+ activated PDS system was introduced in this study for the degradation of acid orange 7 (AO7) dye. The effects of different initial pH, PDS dosage, Fe 2+ dosage, and different UV intensities on the degradation rate of AO7 were investigated, and a kinetic model for the apparent reaction rate was determined. The results showed that the UV/Fe 2+ /PDS system was effective in degrading AO7 in a wide pH range. Under optimal conditions, 96 % removal of AO7 was achieved in 10 min. The effects of different inorganic anions on AO7 were discussed; Cl − had little effect on the degradation effect, and SO 4 2− , NO 3 − and HCO 3 − inhibited the degradation of AO7 by the system to varying degrees. The presence of reactive radicals (SO 4 ·− and·OH) in the reaction was determined by quenching experiments and EPR capture and their degradation contribution was further investigated. Nine intermediates of AO7 were detected by LC-MS/MS, and the degradation pathway of AO7 was inferred by combining with UV-Vis spectra. Finally, the ecotoxicity and tritogenic effects of AO7 intermediates were assessed by Toxtree and T.E.S.T toxicity prediction models, which showed that the final degradation product toxicity was non-mutagenic, non-teratogenic, and devoid of hereditary and non-hereditary carcinogenicity.
研究领域:
环境科学
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化学工程
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毒理学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jiahao Cui,Xiaolong Gao,Kejing Pang,Wenbing Wu,Mrigendra Kumar Awasthi,Yihua Zhao,Xianqiang Yin
Current single-atom studies in the perdisulfate (PDS) system were focused on transition metals, but researching La-series metals might provide new insights for the efficient utilization of this system. The original structure’s Zn was evaporated at high temperatures, thereby we utilized Zeolitic Imidazolate Frameworks (ZIFs) as a substrate to synthesize a type of La-SACs catalysts. The La single atom in this work was identified to the La-N 4 configuration through La-L3 X-ray edge absorption spectroscopy. Experimental observations in suspension demonstrated that the PDS activation capability of La is on par with, if not superior to, that of transition metals such as Co and Cu. Tetracyclines (10 mg/L) were eliminated within 30 min via La-N-C + PDS systems and the pseudo-first-order was higher than 0.0929 min −1 . The Hydrogen bond between PDS and La-N-C and active electron of d orbital in La atoms had the significant influence on the generation of ROS ( 1 O 2 and •OH). Furthermore, the excellent electron transfer of La-N-C also promoted the activation rate of PDS. The findings of this study indicated that La could play a crucial part in PDS catalyst for degradation of organic pollutes in aquatic environment, providing the new method for exploration of single-atom materials in PDS systems.
研究领域:
环境科学
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催化材料
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化学工程
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Yingzi Lin,Junjie Chen,Hao Li,Lei Chen,Baoling Yuan,Chunyan Shi,Siwen Li,Gen Liu,Yuefeng Xie
Acid red 73 (AR73) is a representative dye pollutant that poses a threat to the environment and human health. Effectively removing this type of pollutant by conventional processes is difficult. However, this study found that compared with UV/PDS, UV/O 3 , and PDS/O 3 , UV/O 3 /PDS composite system had the highest degradation effect on AR73. The degradation efficiency in the composite system reached 97.61% within 30 min, and the synergistic coefficients in the composite system were all greater than 1. In the UV/O 3 /PDS system, ·OH was the main free radical that mainly degrades AR73. The increase of PDS dosage promoted the degradation of AR73, but the increase of O 3 dosage was difficult to greatly improve the degradation of AR73 effect. The kinetic model of the apparent reaction rate was determined. The UV/O 3 /PDS system can efficiently degrade AR73 in a wide range of substrate concentrations and pH levels, and at the same time showed good adaptability to various concentrations of anions (Cl − , CO 3 2− , SO 3 2− , and C 2 O 4 2− ). Under raw water quality, the degradation effect of AR73 was still as high as approximately 90%. The theoretical attack site was obtained by DFT calculation , and the possible degradation pathway of AR73 was proposed based on the GC-MS spectrum and UV–Vis absorption spectrum . The attack of –N N- by ·OH, SO 4 − , and O 3 was proposed to be the main possible degradation pathway for AR73. Therefore, this study further improves the understanding of the UV/O 3 /PDS system and shows the potential applicability of this system in the treatment of dye wastewater.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 84
·80595-80603
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IF 3.289
Yang Rong,Liang Tang,Yahui Song,Shengnan Wei,Zhaohong Zhang,Jun Wang
A new visible-light-sensitive photocatalyst, Er3+:Y3Al5O12/MoS2–NaTaO3–PdS, was prepared by hydrothermal, liquid boiling and deposition methods. The prepared photocatalysts were all characterized using an X-ray diffractometer (XRD), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and high-resolution transmission electron microscopy (HRTEM). The photocatalytic activity of the prepared photocatalysts was evaluated via photocatalytic degradation of amaranth as a refractory pollutant with simultaneous hydrogen evolution under visible-light irradiation. Moreover, the effects of the visible-light irradiation time and molar ratio of Er3+:Y3Al5O12 and NaTaO3 on the photocatalytic capability of Er3+:Y3Al5O12/MoS2–NaTaO3–PdS were studied. The results show that the use of Er3+:Y3Al5O12 can improve the utilization ratio of visible light (solar light) for NaTaO3. The optimum ratio of Er3+:Y3Al5O12 and NaTaO3 is 0.45 : 1.00. In addition, a study of extended reusability shows that the prepared photocatalyst can be effectively recycled for three repetitive cycles without an apparent deactivation of the photocatalytic activity. A visible-light photocatalytic degradation mechanism of amaranth with simultaneous hydrogen evolution is also proposed.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
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IF 6.7
Yueli Chen,Huilin Huang,Runying Luo,Aiping Zhang
Landfill leachate contains high levels of refractory organic compounds that pose significant environmental risks. The treatment of landfill leachate through advanced oxidation processes (AOPs) is an effective method for removing these compounds. However, the presence of chloride ions (Cl − ) might lead to the formation of chlorinated organics. In this study, we compared the formation of chlorinated organics during the removal of refractory organic compounds from landfill leachate treated by a membrane bioreactor (MBR) through UV/H 2 O 2 and UV/PDS processes with different oxidant dosages. The relationship between the formation of chlorinated organics and the concentration of organics was explained via ultraviolet visible spectra, three-dimensional excitation and emission matrix spectra, and total organic carbon. The results revealed that the concentration of chlorinated organics increased with increasing oxidant dosage. Under the oxidant dosage of 40 mM and a reaction time of 90 min, the cumulative concentration of the 4 chlorinated organics in the UV/H 2 O 2 process reached 482.8 μg/L, and those of the 8 chlorinated organics reached 34,370.2 μg/L in the UV/PDS process. Concentrations of chloroacetaldehyde, chloroacetic acid and trichloroacetic acid produced in the UV/H 2 O 2 process and concentrations of chloroacetaldehyde, dichloroacetaldehyde and dichloroacetonitrile produced in the UV/PDS process were significantly and positively correlated with the concentrations of aromatic organic compounds. In the UV/H 2 O 2 and UV/PDS processes, the concentration of Cl − affects the conversion of reactive chlorine species, such as Cl • and Cl 2 •– , and the reactive species, such as HO • , SO 4 •– , Cl • and Cl 2 •– generated in the process react with organic compounds to form intermediates through hydrogen extraction, addition and electron transfer processes that gradually open ring structures to form small molecules. Cl • and Cl 2 •– further react with these small-molecule intermediates to form chlorinated organics through chlorine substitution. The toxicity evaluation of chlorinated organics revealed that haloacetaldehydes were the main source of chlorinated organic toxicity in both the UV/H 2 O 2 and UV/PDS processes. This study provides theoretical support for reducing the formation of chlorinated organics during refractory organic compound removal processes from landfill leachate via advanced oxidation processes such as UV/AOPs.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qianlin Ju,Tao Chen,Qianhui Xie,Manli Wang,Kaige Zhao,Tong Liu,Liang Fu,Haozhi Wang,Zelin Chen,Changjiu Li,Yida Deng
As a novel electrochemical energy conversion device, direct ethanol fuel cells are currently encountering two significant challenges: CO poisoning and the difficulty of C–C bond cleavage in ethanol. In this work, an amorphous PdS nanowires/ultrafine IrMnOx bimetallic oxides (denoted as a-PdS/IrMnOx NWs) catalyst with abundant oxide/metal (crystalline/amorphous) inverse heterogeneous interfaces was synthesized via a hydrothermal process succeeded by a nonthermal air-plasma treatment. This unique interfacial electronic structure along with the incorporation of oxyphilic metal has resulted in a significant enhancement in the electrocatalytic performance of a-PdS/IrMnOx NWs toward the ethanol oxidation reaction, achieving current densities of 12.45 mA·cm–2 and 3.68 A·mgPd–1. Moreover, the C1 pathway selectivity for ethanol oxidation has been elevated to 47%, exceeding that of other as-prepared Pd-based counterparts and commercial Pd/C catalysts. Density functional theory calculations have validated the findings that the decoration of IrMn species onto the amorphous PdS surface has induced a charge redistribution in the interface region. The redistribution of surface charges on the a-PdS/IrMnOx NWs catalyst results in a significant decrease in the activation energy required for C–C bond cleavage and a notable weakening of the CO binding strength at the Pd active sites. Consequently, it enhanced both the EOR C1 pathway selectivity and CO poisoning resistance to the a-PdS/IrMnOx NWs catalyst.
研究领域:
材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2017
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IF 0
Zepeng Qu,Yang Rong,Liang Tang,Xiaoqing Shu,Xudong Liu,Zhaohong Zhang,Jun Wang
A new visible-light-induced Z-scheme photocatalytic system, Er 3+ :Y 3 Al 5 O 12 /(MoS 2 /NiGa 2 O 4 )-(BiVO 4 /PdS), is designed and prepared by using hydrothermal and mixed-calcination methods And the prepared samples are characterized by X-ray diffractometer (XRD), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier-transform infrared (FTIR) and UV–vis absorption spectra. The photocatalytic activity is evaluated towards Orange G degradation with simultaneous hydrogen evolution under visible-light irradiation. The photocatalytic experiments indicate that the Er 3+ :Y 3 Al 5 O 12 /(MoS 2 /NiGa 2 O 4 )-(BiVO 4 /PdS) as photocatalyst displays very high photocatalytic activity. It can be ascribed to two sides. One is the use of Er 3+ :Y 3 Al 5 O 12 offering ultraviolet-light to activate the wide-band gap NiGa 2 O 4 . Another is the construction of Z-scheme system between NiGa 2 O 4 and BiVO 4 which can result in a more efficient separation of photoexicited charge carriers, thus endowing it with much powerful oxidation and reduction capabilities. Moreover, the reusability study shows that the prepared photocatalyst can be effectively recycled for three repetitive cycles without an apparent deactivation. In addition, the possible Z-scheme mechanism of Er 3+ :Y 3 Al 5 O 12 /(MoS 2 /NiGa 2 O 4 )-(BiVO 4 /PdS) is also proposed, and further evidenced by photoluminescence (PL) spectra. The present work not only designs a new photocatalytic system but also well applies in photocatalytic degradation of refractory pollutant with simultaneous hydrogen evolution.
研究领域:
环境科学
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材料科学
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光催化技术
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产品关联
DOI
危险品化学品经营许可证（带存储）