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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Optimizing photocatalytic hydrogen evolution performance by rationally constructing S-scheme heterojunction to modulate the D-band center

Zhiliang Jin,Cheng Yang

The research in the field of photocatalysis has progressed, with the development of heterojunctions being recognized as an effective method to improve carrier separation efficiency in light-induced processes. In this particular study, CuCo 2 S 4 particles were attached to a new cubic CdS surface to create an S-scheme heterojunction, thus successfully addressing this issue. Specifically, owing to the higher conduction band and Fermi level of CuCo 2 S 4 compared to CdS, they serve as the foundation and driving force for the formation of an S-scheme heterojunction. Through in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, the direction of charge transfer in the composite photocatalyst under light exposure was determined, confirming the charge transfer mechanism of the S-scheme heterojunction. By effectively constructing the S-scheme heterojunction, the d-band center of the composite photocatalyst was adjusted, reducing the energy needed for electron filling in the anti-bonding energy band, promoting the transfer of photogenerated carriers, and ultimately enhancing the photocatalytic hydrogen production . performance. After optimization, the hydrogen evolution activity of the composite photocatalyst CdS-C/CuCo 2 S 4 -3 reached 5818.9 μmol g −1 h −1 , which is 2.6 times higher than that of cubic CdS (2272.3 μmol g −1 h −1 ) and 327.4 times higher than that of CuCo 2 S 4 (17.8 μmol g −1 h −1 ), showcasing exceptional photocatalytic activity. Electron paramagnetic resonance and in situ X-ray photoelectron spectroscopy have established a theoretical basis for designing and constructing S-scheme heterojunctions, offering a viable method for adjusting the D-band center to enhance the performance of photocatalytic hydrogen evolution.

CAS / MDL: 13963-58-1
研究领域: 材料科学 · 能源化学 · 环境科学
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ChemNanoMat · 2022 ·Vol. 8 ·期 10 ·e202200268 · IF 3.82

Highly Selective Hydrogenation of Nitroaromatics over Pt/TiO2@S-1 catalyst with Inlaid Strong Metal-Support Interaction

Mengmeng Liu,Jingjing Li,Pengfei Wang,Shuai Chen,Zhengping Dong,Fengwei Zhang

Graphical The encapsulation of Pt/TiO 2 -450H catalyst with SMSI into zeolite silicalite-1 (S-1) is reported. The resulting Pt/TiO 2 @S-1 catalyst dispalyed superior catalytic performance especially for halogenated nitroaromatics and without degradation in selectivity after 7 cycles. It is attributed to the high surface area, SMSI effect in confined space and the pore structure of S-1 with selective adsorption of substrates. The encapsulation of metal nanoparticles (NPs)-based active sites and homogeneous catalysts in nanoporous materials has been of highly research focus for tuning their catalytic activity, selectivity and stability. Although the catalysts with strong metal-support interaction (SMSI) hold the reversible encapsulation feature in a certain atmosphere, there is still a lack of systematic research on them in a real confined environment. Herein, we present a highly selective and stable Pt/TiO 2 @S-1 catalyst, which is prepared by in-situ growth of classical silicalite-1 on the external surface of Pt/TiO 2 -450H pre-catalyst with SMSI effect. Encouragingly, the encapsulated 20Pt/TiO 2 @S-1 catalyst demonstrates unprecedented catalytic performance for various nitroaromatics and without any degradation in selectivity after 7 cycles (>99%) for the hydrogenation of 1-chloro-4-nitrobenzene. Such situation is attributed to the high surface area, SMSI effect in confined space as well as the pore structure of silicalite-1 with selective adsorption of substrates.

研究领域: 催化 · 化学工程 · 材料科学 · 环境化学
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CATALYSIS COMMUNICATIONS · 2021 · IF 3.626

Surface gradient diffusion S doping of CuCo2O4 microflowers by an in situ topotactic engineering strategy for CO2 photoreduction

Jianan Li,Wenbo Sun,Xinyong Li,Hangfan Ma,Yaxuan Li,Chong Peng

Photocatalysis is an effective means to convert CO 2 and solar energy into high value-added chemicals. Herein, the surface gradient S doped CuCo 2 O 4 microflowers were fabricated by an in situ topotactic engineering strategy. This photocatalyst presented CO 2 photoreduction with a satisfying activity (5 h, 181 μmol) and stability (94.5% retention). Additionally, the theoretical calculations indicated the fomated M-S bond could be favorbale to facilitate the initial CO 2 ⁎ binding and promote the formation of COOH ⁎ intermediates. This work provides a novel strategy for the fabrication of effective photocatalysts and highlights an in-depth understanding of micro-level regulation towards photocatalytic overall performance.

研究领域: 材料科学 · 化学 · 环境科学 · 纳米技术
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PEST MANAGEMENT SCIENCE · 2023 ·Vol. 79 ·期 8 ·2725-2736 · IF 4.1

Metamifop resistance in Echinochloa glabrescens via glutathione S-transferases-involved enhanced metabolism

Qi Li,Ning Zhao,Minghao Jiang,Mali Wang,Jingxu Zhang,Haiqun Cao,Min Liao

BACKGROUND Echinochloa glabrescens Munro ex Hook. f. is one of the main Echinochloa spp. seriously invading Chinese rice fields and has evolved resistance to commonly used herbicides. Previously, an E. glabrescens population (LJ-02) with suspected resistance to the acetyl-CoA carboxylase (ACCase)-inhibiting herbicide metamifop was collected. This study aimed to determine its resistance status to metamifop and investigate the internal molecular mechanisms of resistance. RESULTS Single-dose testing confirmed that the LJ-02 population had evolved resistance to metamifop. Gene sequencing and a relative expression assay of ACCase ruled out target-site based resistance to metamifop in LJ-02. Whole-plant bioassays revealed that, compared with the susceptible population XZ-01, LJ-02 was highly resistant to metamifop and exhibited cross-resistance to fenoxaprop- P -ethyl. Pretreatment with the known glutathione S -transferase (GST) inhibitor, 4-chloro-7-nitrobenzoxadiazole (NBD-Cl), largely reversed the resistance to metamifop by approximately 81%. Liquid chromatography–tandem mass spectrometry analysis indicated that the metabolic rates of one of the major metabolites of metamifop, N -(2-fluorophenyl)-2-hydroxy- N -methylpropionamide (HPFMA), were up to 383-fold faster in LJ-02 plants than in XZ-01 plants. There were higher basal and metamifop-inducible GST activities toward 1-chloro-2,4-dinitrobenzene (CDNB) in LJ-02 than in XZ-01. Six GST genes were metamifop-induced and overexpressed in the resistant LJ-02 population. CONCLUSION This study reports, for the first time, the occurrence of metabolic metamifop resistance in E. glabrescens worldwide. The high-level metamifop resistance in the LJ-02 population may mainly involve specific isoforms of GSTs that endow high catalytic activity and strong substrate specificity. © 2023 Society of Chemical Industry.

CAS / MDL: 930-55-2 51-03-6
研究领域: 植物科学 · 分子生物学 · 杂草科学
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Water Cycle · 2023 · IF 0

Photocatalytic degradation of sulfamethoxazole over S-scheme Fe2O3/g-C3N4 photocatalyst under visible light

Jiaolong Zhang,Shuting Gou,Zhe Yang,Chaolin Li,Wenhui Wang

The application of promising g-C 3 N 4 has been limited by poor photogenerated electron-hole separation and limited absorption for visible light. Sulfamethoxazole (SMX) is a typical antibiotic drug that is used worldwide and hard to be disposed through conventional wastewater treatment methods. Herein, S-scheme Fe 2 O 3 /g-C 3 N 4 heterojunction was successfully prepared via a facile one-step sintering method and applied to photodegrade SMX under visible light irradiation. The integration of Fe 2 O 3 and g-C 3 N 4 shows superior charge separation and light absorption ability. As a result, the removal efficiency of 11 wt% Fe 2 O 3 /g-C 3 N 4 reaches to 99.2% within 30 min, which is visibly higher than 59.5% of pure g-C 3 N 4 . ·O 2 − and ·OH are demonstrated to be the predominant active species for SMX photodegradation, and the possible degradation pathway is also proposed based on electronic band structure of Fe 2 O 3 /g-C 3 N 4 heterojunction. This study presents a facile construction of g-C 3 N 4 based S-scheme photocatalyst and offers an environmentally friendly approach to effectively remove organic pollutants using renewable solar energy.

研究领域: 环境科学 · 材料科学 · 化学工程
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TRANSACTIONS OF TIANJIN UNIVERSITY · 2012 ·Vol. 18 ·期 5 ·315-319 · IF 0

Synthesis and characterization of novel copolymers based on 3(S)-methyl-morpholine-2,5-dione

Feng Yakai,Chen Chengbin,Zhang Li,Tian Hong,Yuan Wenjie

A series of novel copolymers were successfully synthesized by ring-opening polymerization (ROP) of 3(S)-methyl-morpholine-2,5-dione (MMD) and 5-methyl-5-benzyloxycarbonyl-1,3-dioxan-2-one (MBC) using stannous octoate as catalyst. The copolymers were characterized by means of 1H-NMR and FT-IR spectroscopy. Gel permeation chromatography (GPC) test shows that the average-number relative molecular mass and average-weight relative molecular mass slightly increase with the increase of MBC content in feed. The results of differential scanning calorimetry (DSC) demonstrate that the glass transition temperature of copolymers increases with the increase of MBC content in copolymers. The copolymers of MMD and MBC are amorphous copolymers, as indicated by DSC results, while the homopolymer of MMD is semicrystalline.

研究领域: 高分子化学 · 材料科学
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Journal of Materials Chemistry C · 2015 ·Vol. 3 ·期 34 ·8844-8851 · IF 4.696

Mn2+-doped Zn–In–S quantum dots with tunable bandgaps and high photoluminescence properties

Sheng Cao,Jialong Zhao,Weiyou Yang,Chengming Li,Jinju Zheng

In the present work, we reported the synthesis of Mn2+-doped Zn–In–S quantum dots (QDs) with high optical performance in a controlled manner. The effects of the temperature, the introduced ODE-S amount and Zn/In ratios in the raw materials, as well as the Mn2+ doping concentrations on the photoluminescence (PL) properties of Mn2+-doped Zn–In–S QDs were investigated systematically. The resultant QDs exhibit tunable bandgaps ranging from 2.9 to 3.7 eV, well-resolved Mn2+ d–d emission with a PL quantum yield (QY) of 56% and a surprisingly long excited state lifetime up to ∼4.2 ms, suggesting their excellent PL properties. Meanwhile, the initial high PL QY of the obtained Mn2+-doped Zn–In–S QDs in organic solvents could be preserved very well once they were transferred into aqueous media via ligand exchange. Furthermore, the as-synthesized QDs exhibit excellent thermal stability up to 200 °C in a crude solution.

研究领域: 材料科学 · 光学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Electrospinning directly synthesis of 0D/1D CuBi2O4@WO3 nanofiber photocatalyst with S-scheme heterojunction

Liruhua Zhang,Qianhong Shen,Feilong Huang,Libei Jiang,Jie Liu,Jiansong Sheng,Yue Li,Hui Yang

A novel 0D/1D CuBi 2 O 4 @WO 3 nanofiber-membrane photocatalyst with step-scheme (S-scheme) heterojunction was fabricated by means of the electrospinning method. The disintegration of CuBi 2 O 4 microspheres under a high voltage electrospinning process led to the simultaneous formation of CuBi 2 O 4 nanoparticles on WO 3 nanofibers, therefore constructing well dispersed CuBi 2 O 4 @WO 3 nano-heterojunctions. The CuBi 2 O 4 @WO 3 composite photocatalyst followed the S-scheme charge transfer mechanism, which promoted the efficient charge transfer across the interface, thereby solving the problem that the narrow-bandgap CuBi 2 O 4 had strong light-harvesting ability but easy recombination of photo-generated carriers. Moreover, such S-scheme heterojunction also achieved the spatial separation of photo-induced electrons and holes while ensuring the promising redox abilities in both WO 3 and CuBi 2 O 4 . Hence, the CuBi 2 O 4 @WO 3 composite photocatalyst exhibited excellent photocatalytic activity for photocatalytic degradation of antibiotics in environmental remediation under weak-visible-light irradiation (5 W LED lamp), and its photocatalytic activity for tetracycline degradation was significantly improved, which was 8.1 times and 3.6 times than that of WO 3 nanofibers and pure CuBi 2 O 4 microspheres, respectively. The radical species trapping tests indicated that·O 2 − and h + were the main active radicals in the tetracycline photodegradation reaction, and the high-performance liquid chromatography-mass spectrometry test clarified three possible degradation reaction pathways of tetracycline. This work presented a facile method to fabricate 0D/1D CuBi 2 O 4 @WO 3 composite nanofiber photocatalyst with well-dispersed CuBi 2 O 4 @WO 3 nano-heterojunctions, and also provided a new idea for the preparation of new nanocomposite photocatalyst based on electrospinning process.

研究领域: 环境科学 · 材料科学
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Laser & Photonics Reviews · 2023 ·Vol. 18 ·期 1 ·2300809 · IF 11

Multinary Cu─In─Zn─S-based Quantum-Dot Electroluminescence and Implications on Device Designs

Xiankun Zheng,Lijin Wang,Jialin Bai,Han Zhang,Hanzhuang Zhang,Aiwei Tang,Wenyu Ji

Currently, the performance of quantum-dot light-emitting diodes (QLEDs) based on environmental-friendly Cu─In─Zn─S quantum dots (QDs) still lags far behind that of Cd-QDs-based devices. Here it is demonstrated that the unique trap-related recombination in Cu─In─Zn─S QDs is mainly responsible for the low device efficiency. The luminous efficiency of Cu─In─Zn─S-based QLEDs is rather sensitive to the temperature and hole-transporting layers (HTLs) due to the susceptible thermal-related trappingdetrapping processes of holes in radiative Cu-related traps. The holes in Cu-related traps can be quenched by escaping to the valence band of the QDs or/and transferring to the adjacent HTLs. An HTL with low highest occupied molecular orbitals is desired to enhance the hole injection and hinder the aforementioned hole transfer. As a result, a high device efficiency of 6.0 cd A −1 is achieved at room temperature, which is attributed to suppressed HTL-induced emission quenching and efficient valence-band-dominated hole injection from HTL to the QDs. The device efficiency is further increased to 13.2 cd A −1 at 150K by suppressing thermal-induced quenching.

研究领域: 材料科学 · 光电技术
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MOLECULES · 2024 ·Vol. 29 ·期 9 ·1931 · IF 4.2

Preparation of S-C3N4/AgCdS Z-Scheme Heterojunction Photocatalyst and Its Effectively Improved Photocatalytic Performance

Yuhong Lin,Zhuoyuan Chen,Chang Feng,Li Ma,Jiangping Jing,Jian Hou,Likun Xu,Mingxian Sun,Dongchu Chen

In this study, S-doped graphitic carbon nitride (S-C3N4) was prepared using the high-temperature polymerization method, and then S-C3N4/AgCdS heterojunction photocatalyst was obtained using the chemical deposition method through loading Ag-doped CdS nanoparticles (AgCdS NPs) on the surface of S-C3N4. Experimental results show that the AgCdS NPs were evenly dispersed on the surface of S-C3N4, indicating that a good heterojunction structure was formed. Compared to S-C3N4, CdS, AgCdS and S-C3N4/CdS, the photocatalytic performance of S-C3N4/AgCdS has been significantly improved, and exhibits excellent photocatalytic degradation performance of Rhodamine B and methyl orange. The doping of Ag in collaboration with the construction of a Z-scheme heterojunction system promoted the effective separation and transport of the photogenerated carriers in S-C3N4/AgCdS, significantly accelerated its photocatalytic reaction process, and thus improved its photocatalytic performance.

CAS / MDL: 81-88-9
研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

The role of Cu0 in propane dehydration over extremely-low loaded PtCu@S-1 catalyst

Kai An,Hongyan Jia,Ruobing Cheng,Yong Guo,Xiaohui Liu,Yanqin Wang

Pt-based bimetallic catalysts have gained more and more attention in propane dehydrogenation (PDH), but still suffer from the high cost and poor stability. In this work, a PtCu@S-1 catalyst with an extremely low loading of Pt (0.047 wt%) is prepared by in-situ hydrothermal synthesis and employed in PDH. An excellent productivity (propylene yield: 471.8 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 ) is achieved at 600 °C with a weight hour space velocity of 25.80 h −1 . After 50 h of reaction at 600 ℃, 0.047Pt0.19Cu@S-1 catalyst still remains sinter-free, with a deactivation rate of only 0.006 h −1 . Various characterizations show that Cu 0 co-existed with Pt 0 in PtCu@S-1 catalyst plays an important role, greatly improved catalyst reactivity and stability. At high weight hour space velocity (44.5 h −1 ), the propylene productivity can reach 1056.4 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 . This work provides a new way for the design of extremely low Pt-loaded PDH catalysts with excellent performance at high temperatures.

CAS / MDL: 7758-99-8
研究领域: 催化化学 · 材料科学
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Journal of Materials Chemistry C · 2019 ·Vol. 7 ·期 5 ·1307-1315 · IF 6.641

Seeded-mediated growth of ternary Ag–In–S and quaternary Ag–In–Zn–S nanocrystals from binary Ag2S seeds and the composition-tunable optical properties

Bin Zeng,Fei Chen,Zhenyang Liu,Zhongyuan Guan,Xu Li,Feng Teng,Aiwei Tang

Herein, we demonstrated a seed-mediated growth method for the synthesis of ternary AgInS2 (AIS) and quaternary Ag–In–Zn–S (AIZS) nanocrystals (NCs) by means of a partial cation exchange with In3+ and Zn2+ ions. Binary Ag2S NCs with different sizes were synthesized first, which then acted as the seeds to prepare different-sized AIS NCs through the incorporation of In3+. The formation mechanism of AIS NCs was studied in terms of the temporal evolution of the morphology and crystal structure, and the heterostructured Ag2S-AIS NCs were formed as intermediates during the growth process of AIS NCs. Variation in the Ag/In feeding ratios from 1 : 1 to 1 : 3 led to a broad tuning of the optical band gap and photoluminescence (PL) maximum of AIS NCs, in which very small-sized AIS NCs with a tetragonal phase were obtained. Subsequently, the incorporation of Zn2+ into AIS NCs resulted in the widening of the optical band gap and the shift of the PL maximum to higher energy with the enhancement of the absolute PL quantum yields (PLQYs). When the reaction temperature was increased, the PL emission maximum could be tuned from 2.04 to 2.33 eV and the absolute PLQYs could be tuned from 16% to 58%. Time-resolved PL spectroscopy was used to study the PL decay dynamics of the AIS and AIZS NCs, and the PL emission was related to the recombination of the surface-related states, intrinsic defects and donor–acceptor (D–A) pairs. The ternary and quaternary Ag-based semiconductor NCs have long-lived excitons, which may have promising applications in the field of energy conversion.

研究领域: 材料科学 · 纳米技术 · 光学
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