CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiarun Cheng,Chaojie Lyu,Hongming Chen,Dongsheng Geng,Jinlong Zheng
Elucidating the mechanism of metal-support interface domain regulation is crucial for designing efficient fuel cell electrocatalysts. Herein, we propose an emerging strategy to enhance oxygen reduction reaction (ORR) activity and selectivity by regulating the Lewis alkalinity of carbon support to adjust the Lewis acidity of metal sites. The experimental results and density functional theory (DFT) simulations show that the introduction of N/S atoms into the carbon support structure will break the charge balance of the carbon skeleton and effectively regulate the charge distribution in the Pt-carbon interface domain, thus promoting the oxidation of the Lewis acid Pt atoms to a higher valence state Pt x+ , so as to optimize the adsorption energy of oxygen-containing intermediates. Moreover, Bader charge analysis also verifies that N,S-HMCS, as a Lewis base, can receive more electrons from the Pt sites of Lewis acid, and the electron loss at Pt sites caused by N,S-HMCS strengthens interfacial electron effect. Meanwhile the strong electron adsorption ability of N/S atoms causes the d-band center of Pt atom orbital to shift upward to the Fermi level, which strengthens the binding of metal Lewis acid Pt sites with *OOH intermediates, and improves the 4-electron transfer mechanism. This research reveals the direct role of Lewis acid sites in ORR of fuel cell cathode, and provides a feasible way to guide the design of electrocatalysts with Lewis acid/base double centers.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Yang Yu,Lichao Xu,Kaiyuan Xu,Yan Li,Hao Chen,Dongxu Zhang,Yuanzi Chen,Yue Liu,Wenyue Qi
The construction of S-scheme heterojunctions has drawn widespread attention within the photocatalysis field due to their capacity for efficient separation of photogenerated carriers, leading to excellent photo-oxidation-reduction performance. Herein, a novel S-scheme loofah biochar/MoS 2 /g-C 3 N 4 (LB/MS/CN) heterojunction was successfully constructed by ultrasonication in 50 % ethyl alcohol and heat treatment in N 2 atmosphere. Degradation experiments showed that the 5 % LB/MS/CN ternary photocatalyst had optimal photocatalytic efficiency (96.4 %) for the degradation of rhodamine B (RhB), and the reaction rate (k) of this photocatalyst (0.05420 min −1 ) was 5.4 times that of unmodified CN (0.01001 min −1 ). Ultraviolet-visible diffuse reflectance spectra, Mott-Schottky, and free radical trapping experiments suggested that the photogenerated carriers in LB/MS/CN were transferred through the S-scheme structure. Consequently, the co-catalytic action of LB and the synergistic impact of the heterojunction structure between CN and MS led to a reduced photogenerated carrier recombination rate. Furthermore, LB/MS/CN had outstanding stability and the capacity to maintain RhB degradation performance under various environmental conditions (H 2 PO 4 − , NO 3 − , SO 4 2− , HCO 3 − , NaCl, humic acid (HA), and real water), showing good promise for practical applications. Thus, this work provides a possible strategy for purifying wastewater under visible light.
研究领域:
环境科学
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材料科学
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光催化
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产品关联
DOI
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2023
·Vol. 52
·期 8
·5422-5429
·
IF 2.1
Xu Jiaxiong,Wu Xiaoshuai
Chalcogenide Cu 2 ZnSn(S,Se) 4 (CZTSSe) is a promising absorber material for photovoltaic applications. When CZTSSe thin film is deposited on an Mo substrate, a Mo(S,Se) 2 layer easily forms between the CZTSSe and the Mo, which is detrimental to the back contact property of the CZTSSe. This work proposes a useful way to inhibit the formation of Mo(S,Se) 2 by sputtering a CuCrO 2 layer on a Mo-foil substrate before the deposition of the CZTSSe. The effects of CuCrO 2 thickness on the crystalline structures, morphologies, and electrical properties of the fabricated samples were studied. The results showed that the insertion of the CuCrO 2 layer prevented the formation of Mo(S,Se) 2 . As the thickness of the CuCrO 2 increased, the thickness of the Mo(S,Se) 2 layer decreased. The Mo(S,Se) 2 layer was absent from the cross-sectional scanning electron microscopy image when the CuCrO 2 thickness exceeded 85 nm. The back contact resistance of CZTSSe decreased monotonously as the CuCrO 2 layer thickened due to the reduction in the Mo(S,Se) 2 layer thickness. Therefore, by inserting a CuCrO 2 layer to separate the CZTSSe and the Mo-foil, the formation of the Mo(S,Se) 2 layer between them was effectively suppressed, and the back contact properties of the CZTSSe thin film were significantly enhanced.
研究领域:
材料科学
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光伏技术
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薄膜太阳能电池
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Gongcheng Sun,Subing Fan,Junmin Lv,Tiansheng Zhao
A hollow zeolite encapsulated Rh catalyst Rh@H-S-1 with an “eggshell” structure was prepared using the method of organic alkali treatment and recrystallization. Compared with catalysts with directly encapsulated Rh@S-1 and surface impregnated Rh/S-1, this catalyst exhibited both superior activity and a higher TOF value in hydroformylation of 1-hexene due to the high dispersion of Rh and high diffusion. The Rh element did not need to be reduced in the preparation, and it was in situ reduced by the syngas. The content of lower valence Rh δ+ gradually increased with the reaction procedure and played as an active center. The low oxidized state Rh + or Rh δ+ in the form of Rh(CO) 2 are proposed as active sites in hydroformylation, which were generated under the synergistic effect between CO and H 2 . Importantly, the hollow encapsulated catalyst effectively decreased Rh leaching to 0.1 ppm and showed better stability compared with the impregnated Rh/S-1 catalyst.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Xinyi Chi,Mingyu Dou,Guang Yang,Ruixin Yang,Zunhao Wang,Hengyi Wang,Hua Yang,Wenning Yang,Erkang Liu,Jianmin Dou
The development of efficient and durable non-noble metal photocatalysts remains a major challenge, primarily owing to the fast recombination of photogenerated charge carriers and sluggish interfacial reaction kinetics. In this work, a ternary composite photocatalytic system, CdLa 2 S 4 /Mn 0.5 Cd 0.5 S-Co x P (CdLa 2 S 4 /MCS-Co x P), was rationally designed and constructed by coupling the S-scheme heterojunction with the metal-semiconductor Schottky interface, aiming to synergistically enhance multi-channel charge separation and migration. The construction of an S-scheme heterojunction comprising CdLa 2 S 4 and Mn 0.5 Cd 0.5 S (MCS) significantly facilitates the spatial separation of photogenerated electrons and holes driven by the built-in electric field, while simultaneously preserving their strong redox capability. Meanwhile, the Co x P acts as both an efficient electron acceptor and proton reduction site, its Schottky barrier at the interface further lowers the energy barrier for the hydrogen evolution reaction and accelerates surface reaction kinetics. Consequently, the CdLa 2 S 4 /MCS-Co x P composite exhibits a remarkable hydrogen evolution rate of 11.04 mmol g −1 h −1 , outperforming pristine MCS and CdLa 2 S 4 by factors of 10.32 and 38.07, respectively. This study offers a practical strategy for the rational design of multi-interface photocatalytic architectures with robust redox ability.
研究领域:
材料科学
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催化
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纳米技术
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能量转换
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半导体物理
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 51
·2208676
·
IF 19.924
Bo Pang,Zuquan Jin,Yunsheng Zhang,Zhiyong Liu,Wei She,Penggang Wang,Yong Yu,Xiaoying Zhang,Chuansheng Xiong,Ning Li,Guowen Sun,Peng Zhao,Guojian Liu,Xiaoyun Song,Song Gao
Cement-based sensors (CBSs) have demonstrated potential in structural health monitoring (SHM) despite rare applications due to their poor flexibility and sensing accuracy/protection with robustness. Herein, a promising strategy is reported to design a waterborne epoxy resin (WEP)-modified cement-based composite coating sensorcapable of simultaneous stable SHM and durable protection. The interpenetrating network (IPN) formed by WEP within cement paste is bionic to the toughness and crack resistance of biological muscle tissue and balances the ion permeation performance and polarization of hydration products. The polymerization-redispersion progress and mechanism of calcium silicate hydrate (C-S-H) gel modified with [3-(2-aminoethylamino)-propyl]trimethoxysilane silsesquioxane (C-POSS) are characterized and revealed. The results show that the muscle-like IPN increases the cement-based coatings’ maximum deflection angle to 30° and improves the monitoring accuracy of compressive, tensile, and fatigue microchanges of concrete structures to more than 95%. The POSS···Ca 2+ ···C-S-H interaction in C-POSS partially transferred the intra-adhesive hydrogen bonds surrounding the nanoconducer into electrostatic bridging ones to maintain an excellent electromechanical conductive dispersion.
研究领域:
土木工程
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材料科学
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传感器技术
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Zhuo Liu,Chao Xiong,Lin Gan,Junhui Yin,Xueying Wang,Jintao Li,Jiayi Wang,Jintong Li,Changyu Lu
In this work, the S-scheme MnFe 2 O 4 /ZnIn 2 S 4 (MFO/ZIS) heterostructure was prepared by hydrothermal method, which can degrade tetracycline (TC) and 2,4,6-trinitrotoluene (TNT) efficiently. Under simulated sunlight irradiation, 88.9 % of TC can be degraded within 75 minutes, and 82.7 % of TNT can be degraded within 120 minutes. The photocurrent response of 3 %MFO/ZIS (0.45 µA cm- 2 ) surpassed that of ZIS (0.15 µA cm −2 ) and MFO (0.08 µA cm −2 ). This is mainly due to the synergistic effect of the S-scheme electron transport pathway and the photothermal effect in MFO/ZIS, which improves its utilization rate of photogenerated electrons. After being used four times, 3 %MFO/ZIS can still degrade 80.2 % of TC, showing excellent stability. In addition, the TC degradation process was analyzed and the low toxicity of TC after degradation was confirmed by LC-MS, ECOSAR and experiments of cultivating mung bean sprouts, demonstrating the potential application value of MFO/ZIS heterojunction in the wastewater treatment field.
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
ChemistrySelect
·
2025
·Vol. 10
·期 1
·e202403867
·
IF 2
Ben Liu,Binghong Wu,Lianghui Chen,Xinxin Zhang,Jinguo Lin,Xiaoyun Chen
Graphical A cellulose-supported SnW(S,O) 4 bimetal sulfo-oxide catalyst (SW@C) with exceptional catalytic activity in the reduction of MB, RhB, and Cr(VI) in the presence of NaBH 4 under dark conditions were synthesized, which is significant for advancing future research on environmental pollution management using biomass-based materials. In this paper, cellulose-supported SnW(S,O) 4 bimetal sulfo-oxide catalysts (labeled as SnWSO-C or SW@C) with exceptional catalytic performance in the reduction of MB, RhB, and Cr(VI) in the presence of NaBH 4 under dark conditions were synthesized via an in-situ hydrolysis method. The cellulose-supported catalyst system with diverse tree species of Pinus massoniana (Pm), Populus tomentosa Carrière (Ptc), Rice hull (Rh), Phyllostachys edulis (Pe) was investigated. The 100 mL solutions of MB (20 ppm), RhB (50 ppm), and Cr(VI) (50 ppm) were completely reduced by SW@Cotton, SW@Pe, SW@Rh, SW@Ptc, and SW@Pm within 10, 7, 13, 4, and 4 min for MB; 7, 7, 8, 10, and 4 min for RhB; and 5, 8, 10, 10, and 8 min for Cr(VI), respectively. Among them, SW@Pe catalyst exhibits the highest catalytic reduction efficiency and excellent stability, maintaining a removal rate of 96% after six cycles. The superior catalytic reduction performance was attributed the unique properties of Phyllostachys edulis cellulose, characterized by low crystallinity (53.25%), minimal ash content (0.15%), and the lowest degree of polymerization (1267). These features facilitated the improved dispersion of the SnWSO bimetal sulfo-oxide, leading to smaller crystal size, lower electrochemical impedance (2.24 Ω), and a larger electrochemically active surface area (21.86 mF/cm 2 ). This study demonstrates the potential of cellulose-supported bimetal sulfo-oxide catalysts for wastewater treatment, which is significant for advancing future research on environmental pollution management using biomass-based materials.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuyan Wang,Hongxia Zhang,Wei Gao,Ming Zhong,Bitao Su,Ziqiang Lei
In this work, two series of plasmonic S-type heterojunction photocatalysts containing Bi, TiO 2 , and biochar (Bi/TiO 2 @C) have been developed through a biomass-assisted hydrothermal-calcination strategy, utilizing grapefruit peel as a reducing agent and C resource. The calcination temperature and the mass ratio of biomass were optimized to obtain the optimal nanocomposite, which shows excellent adsorptive and visible-light photocatalytic performance in the removal of diverse antibiotic and dye pollutants, including tetracycline, oxytetracycline, ciprofloxacin, sulfamethoxazole, sulfisoxazole, malachite green, and rhodamine B. The remarkable performance can be attributed to the enhanced absorption of light absorption resulting from the localized surface plasmon resonance effect of the semimetal Bi, and the formation of heterogeneous interface between Bi and TiO 2 , which accelerates the transfer of photogenerated charge. Furthermore, trapping tests and electron spin resonance (ESR) analysis reveal that ∙O 2 - and h + are the primary active species involved in the removal of tetracycline. A plausible charge transfer mechanism has been proposed.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Chuantao Wang,Xiang Li,Xueting Lv,Xin Huang,Yueyue Zhao,Tiantian Deng,Jiale Zhang,Jun Wan,Yanzhong Zhen,Tuo Wang
The construction of S-scheme heterojunction with excellent redox ability holds promising prospects for photocatalytic environment remediation. However, the rationally design of the heterojunction interface to achieve efficient charge transfer still faces challenges. In this study, we fabricated a tight-contacted S-scheme heterojunction by in situ anchoring AgI nanoparticles onto WO 3 nanoplates. The significant difference in Fermi energy levels between WO 3 and AgI results in the formation of a space charge region around the interface and bending of the energy band, facilitating directional migration and spatial separation of charge carriers. This contributes to enhanced generation of superoxide radicals (•O 2 − ) and holes (h + ) active species, leading to a significant increase in chlortetracycline (CTC) degradation rate. The apparent rate constant for CTC removal using the WO 3 /AgI (WA-2) is approximately 15 times higher than that observed for pure WO 3 . Furthermore, WA-2 exhibits universal degradation effects on tetracycline (TC) and oxytetracycline (OTC). Molecular dynamics (MD) simulation reveals the synergistic adsorption effect of WO 3 and AgI on CTC and reactive oxygen species molecules. Based on Fukui function calculation of CTC molecules and degradation intermediates, liquid chromatography-mass spectrometry (LC-MS) analysis, photocatalytic degradation pathway over WO 3 /AgI was determined to be sequential demethylation followed by dechlorination and decarbonylation. These findings provide valuable insights into high-performance S-scheme heterojunctions interface design and elucidation of pollutant degradation mechanism.
研究领域:
环境科学
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材料科学
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计算化学
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产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 10
·103504
·
IF 3.9
Lu Chen,Qibin Tao,Lin Wang,Hao Lan,Qizhou Dai
In this study, a lead dioxide electrode co-modified with carbon microspheres and neodymium (CMS-Nd-PbO2) was prepared. The structural morphology and electrochemical properties of the four electrodes, PbO2, CMS-PbO2, Nd-PbO2, and CMS-Nd-PbO2, were compared by field emission scanning electron microscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, cyclic voltammetry, and electrochemical impedance, respectively. The results showed that the prepared CMS-Nd-PbO2 electrode had higher surface denseness and higher electrode activity. Based on the accelerated lifetime experiment, the actual working life of four electrodes was studied, and the CMS-Nd-PbO2 electrode had a relatively long lifetime, increased 24.60% compared with the PbO2 electrode. The influencing parameters of electrochemical degradation of bisphenol S (BPS) by CMS-Nd-PbO2 electrode, the ability of different electrodes to generate hydroxyl radicals, reaction mechanism, and the possible BPS degradation pathways were also discussed. Further, the safety of the prepared electrode was evaluated. Under the optimal parameters, the removal rate of BPS and chemical oxygen demand (COD) were 96.49% and 51.84%, respectively. The dissolved lead ion concentration in the solution after electrochemical oxidation was lower than the WHO standard. The CMS-Nd-PbO2 electrode showed promising applications in the degradation of emerging contaminants wastewater.
研究领域:
环境科学
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电化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xinyue Duan,Yingqing Zhan,Hongshan Jia,Jie Liu,Yajie Lei,Jing Yang,Yuxing Han
MXene nanosheets based membrane materials encounter challenges in the field of oil-water separation, including narrow interlayer spacing, insufficient stability, and limited photocatalytic self-cleaning efficiency. To address the aforementioned issues, the 2D/2D MXene nanosheets based heterojunction was constructed through in situ growth of porous ZnIn 2 S 4 and freely assembled onto a PAN fibrous membrane with via vacuum-assisted self-assembly technology. The resulting MXene/ZnIn 2 S 4 @PAN fibrous composite membrane (FCM) exhibited high flux and exceptional photocatalytic self-cleaning property. On the one hand, the porous petal-like structure and intrinsic hydrophilic nature of MXene/ZnIn 2 S 4 heterojunction offered the remarkable nanochannel modulation capability, enabling the composite membrane to achieve high permeability (5471.13 -6732.57 L m -2 h -1 ) compared with the conventional MXene based composite membranes with compacted lamellar structure. On the other hand, the heterojunction formed between MXene and ZnIn 2 S 4 significantly improved electron conduction efficiency and effectively regulated the energy band structure, as confirmed by electrochemical impedance spectrum and UV–visible near infrared diffuse reflection test. This imparted the composite membrane with exceptional photocatalytic self-cleaning capability for the degradation of organic dyes, with the degradation efficiency reaching as high as 92.15%. Besides, the rational photocatalytic mechanism was proposed on the basis of free radical quenching and EPR experiments. Such high-flux and enhanced self-cleaning PAN FCM showed the potential in dealing with complicated membrane fouling issues and separating emulsified oily wastewater.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
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