NEW CARBON MATERIALS
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2024
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IF 6.5
Tan Yi,Jun-long Huang,Zong-heng Cen,Yi-wei Ji,Shao-hong Liu
Carbon-based catalysts are promising materials for the electrochemical extraction of uranium from seawater. However, their practical application is often limited by high cost and low catalytic activity. Using low-cost polystyrene sulfonic acid resin and melamine as raw materials, a class of nitrogen and sulfur co-doped carbon nanosheets (CNSs) with high catalytic activity has been developed by a low-temperature hydrothermal treatment and high-temperature carbonization. Because of their high conductivity and high catalytic activity, CNS-based electrodes can catalyze uranyl ions in seawater into easily recoverable Na 2 O(UO 3 ·H 2 O) x precipitates at −2 V, and achieve an extraction capacity of up to 3 923.7 mg g −1 with a uranium removal of 98.1% in uranium-spiked seawater (1×10 3 mg L −1 ). In situ Raman spectroscopy showed that a large number of uranium compounds appeared on the surface of the composite electrode within 40 min of extraction. The electrode also recovered 72.7% of the uranium in natural seawater, demonstrating excellent prospects for this application. This work provides a new approach into the design of low-cost, metal-free electrocatalysts for the efficient uranium extraction from natural seawater.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Haobin Song,Tong Li,Tingting He,Zhouhao Wang,Daliang Fang,Ye Wang,Xue Liang Li,Daohong Zhang,Junping Hu,Shaozhuan Huang
The intelligent design of catalytic materials with unique architectures has a significant impact on regulating the polysulfides (LiPSs) conversion and boosting the performance of Li − S batteries. Here, starting from 2D catalytic MoS 2 nanosheets and combined with the first-principle calculations, the covalent heterojunction and S vacancy are simultaneously developed in MoS 2 to regulate the electronic structure and improve the LiPSs conversion kinetics. The S vacancy and heterojunction (MoS 2-x -Co 9 S 8-y ) engineering can significantly improve the electrical conductivity of MoS 2 by incorporating shallow donor levels into the MoS 2 . Moreover, the incorporation of Co 9 S 8-y greatly improves the chemisorption ability of heterostructure towards LiPSs. The LiPSs are preferentially adsorbed at the catalytic Mo-S-Co heterojunction, where both Li + and e - are easy to access. The coupled fast Li + /e - transportation of MoS 2-x -Co 9 S 8-y enables direct and fast LiPSs “adsorption-conversion” at the catalytic Mo-S-Co heterojunction with enhanced bidirectional catalytic properties. Due to the ingenious co-engineering of S vacancy and heterointerface, the Li − S cell with MoS 2-x -Co 9 S 8-y /rGO interlayer delivers high sulfur utilization (1382.5 mAh/g at 0.1C), excellent rate capability (710.2 mAh/g at 3C), and long cycle life over 600 cycles (0.06 % capacity decay per cycle). This work demonstrates the great potential of anion deficiency and heterojunction co-construction for high-performance Li − S batteries.
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FUEL
·
2024
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IF 6.7
Man Lang,Dengwei Wang,Shenbo Yang,Hao Li
The development of excellent performance catalysts for the hydrodeoxygenation of renewable biomass into value-added chemicals is essential but remains extremely challenging. Herein, a series of novel metal-free carbo-catalyst catalysts through one-step-pyrolysis strategy were fabricated for the hydrodeoxygenation (HDO) of lignin-derived vanillin (VAN) to produce 2-methoxy-4-methylphenol (MMP). It has been demonstrated that 81.32 % VAN conversion could be acquired with a high selectivity of 77.30 % of MMP under the condition of 240 °C, 1 MPa H 2 and 4 h with the assistance of the optimized NSCC-800-7 catalyst. After characterization of the catalyst and density functional theory (DFT) calculations, the outstanding catalytic activity is attributed to the synergistic effect between nitrogen and sulfur dopants, which effectively regulates the number of active sites. N-S vacancy (NSVs) in the N-doped carbon catalysts is found to play an active site for the VAN HDO reaction, which is greatly beneficial to activating hydrogen molecules. Meanwhile, sulfur doping can promote the formation of defect sites and high specific surface area, while enabling to stabilization of NSVs. Additionally, isopropanol was both the reaction medium and the secondary hydrogen donor, which contributed to reducing the external hydrogen supplication. This finding can open broad opportunities for the rational design of novel metal-free catalysts for challenging chemical reactions.
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Materials Today Chemistry
·
2024
·
IF 6.7
Xiangfeng Sun,Xuan Song,Dongxia Li,Yuxin Xue,Yulin Fu,Yuanhao Shi,Zhiqi Li,Chongxian Luo,Qiong Lin,Xuefeng Gui,Jiwen Hu,Kai Xu
Lithium-sulfur batteries (LSBs) have been considered as ideal candidates for next-generation energy storage equipment. However, its development has been hindered by the shuttle effect exhibited by the intermediate lithium polysulfides (LiPSs). To address this problem, covalent organic frameworks (COFs) show great promises as sulfur hosts for LSBs. We devised and synthesized a covalent organic framework (TPAS–TPB–COF) that is rich in redox sites by solution polymerization. The reactive groups in the covalent organic framework nano–channels not only inhibit the shuttling of polysulfides, but also promote the migration of Li ions. Meanwhile, the abundant cavities as well as redox sites in the COF nano–channels achieve a high sulfur loading capacity (∼71 wt%), a strong LiPS adsorption capacity, and facilitate ion diffusion. Based on these advantages, when it is used as a sulfur host for LSBs, our COF system provides a high capacity of 1134 mAh g −1 at 0.2 C (1 C = 1675 mA g −1 ), an outstanding rate capability (560 mAh g −1 at 4 C), and excellent stability.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2024
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IF 6.3
Yu He,Chenxi Zhao,Zecheng Lu,Ning Guo,Hongmei Luan,Yanchun Yang,Ruijian Liu,Chengjun Zhu
Indium tin oxide (ITO) and intrinsic ZnO (i-ZnO) are usually used as the window layer of Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cells within a typical structure. The optoelectronic properties of the window layer play a crucial role in determining the efficiency of solar cells. In this work, two types of CZTSSe solar cells with and without i-ZnO layers were fabricated using dimethyl sulfoxide (DMSO) and dimethylformamide (DMF) as solvents, respectively. The impact of the window layer on the performance of CZTSSe solar cells was investigated. The results suggest that the device without i-ZnO still exhibits a high power conversion efficiency (PCE) compared to conventional bilayer i-ZnO/ITO structures. By removing i-ZnO and optimizing the thickness of ITO, the highest power conversion efficiency (PCE) of DMSO and DMF-based CZTSSe solar cells has been up to 10.17% and 10.27%, respectively, with an increase in open-circuit voltage (V OC ) of 15 mV (in DMSO system) and 10 mV (in DMF system), as well as an enhancement in fill factor (FF) by ∼5 percentage points. These performance improvements are mainly attributed to the reduction of series resistance (R s ) of the window layer due to the removal of i-ZnO layer. Further analysis shows that the generation and collection of photon-generated carriers in CZTSSe solar cells can be affected by the optimized window layer due to optical interference effects and its resistance. Our research may provide insights for the preparation of high efficient CZTSSe solar cells with new structures of the i-ZnO free window layer.
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Journal of Energy Storage
·
2025
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IF 9.8
Lu Zhong,Yuejia Qin,Zenan Zhou,Lianyun Zhong,Jietian Liang,Shaohui Hu,Qifan Liu,Yanfei Zeng,Shunmin Yi,Hui You,Shengkui Zhong,Dongliang Yan
Olivine-type lithium iron phosphate (LFP) serves as a prominent cathode material for Li-ion batteries, attributed to its natural abundance, remarkable cycling stability, eco-friendliness, and cost-effectiveness. Nonetheless, its additional utilization has been constrained by its inherent low conductivity and sluggish lithium-ion diffusion rate. Incorporation of heteroatom-doped carbon coatings serves as an effective method to enhance the electrochemical properties of LFP, leading to a notable improvement in both the electronic and ionic conductivity of the material. At present, however, the preparation of heteroatom-doped carbon cladding layer is mostly done by secondary sintering method, which is too cumbersome. In this paper, lithium iron phosphate containing N- and S-element doped carbon layers is synthesized by a simple one-step ball milling method using zein as a source of carbon layers and heteroatoms. The results show that the N- and S-doped carbon-coated lithium iron phosphate prepared from zein has lower polarization by enhancing the diffusion kinetics of the lithium-ion battery. NS/C15@LFP shows an initial discharge specific capacity of 155.97 mAh·g −1 at 0.1C and still shows 84.06 mAh·g −1 at 20C. After returning to 0.1C, there is still a discharge capacity of 161.4 mAh·g −1 . The capacity retention rate is 87 % after 500 cycles at 1C and 89 % after 500 cycles at the high current density of 5C, suggesting its excellent electrochemical performance. This work shows that lithium iron phosphate coating N- and S-doped carbon synthesized by using zein as the carbon source and heteroatom donor is a simple and low-cost strategy that gives LFP excellent electrochemical performance.
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Small
·
2024
·
IF 13
Shikai Wang,Dong Zhang,Xipeng Pu,Lizhi Zhang,Dafeng Zhang,Jizhou Jiang
Herein, guided by the results of density functional theory prediction, the study rationally designs a hollow core–shell FeNi 2 S 4 @ZnIn 2 S 4 (FNS@ZIS) Step-scheme (S-scheme) heterojunction for photocatalytic H 2 evolution with photothermal-assisted. The hollow FNS spheres offered substrate for coating the ZIS nanosheets, which can inhibit ZIS nanosheets from agglomerating into pellet, enrich the active site, increase specific surfaces, and raise the light absorption. Notably, due to its excellent photothermal properties, FNS core generated heat unceasingly inside under visible-light irradiation and effectively prevent the heat loss of the reaction system, which increased the local temperature of photocatalysts and thus accelerated the charge migration. In addition, the S-scheme heterojunction construction via in situ growth has a tight interface, which can facilitate the separation and transfer of carriers and achieve high redox potential. Owning to the distinctive construction, the hollow core–shell FNS@ZIS S-scheme heterojunction show extraordinary stability and photocatalytic H 2 evolution rate with 7.7 mmol h −1 g −1 , which is ≈15.2-fold than pristine ZIS. Based on the double evidence of theoretical predictions and experimental confirmations, the photothermal effect and electron transfer mechanism of this innovative material are investigated in depth by the following infrared thermography technology and deep DFT calculations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Wenting Li,Zhuoran Yang,Chunyu Yang,Wei Guo
This study addresses the challenge of enhancing ferroptosis efficacy for tumor therapy, particularly the limited therapeutic efficiency of current inducers due to tumor microenvironment constraints. Herein, we developed a hollow ultrasound-triggered ZnFe 2 O 4 -Bi 2 MoO 6 (ZB) S-scheme heterojunction loaded with artesunate (ART) to overcome these limitations. The ZB heterojunction with a particle size of ∼250 nm efficiently separates electron-hole pairs under ultrasound (US), promoting the generation of reactive oxygen species (ROS). The photodynamic effect of ZB further boosts ROS production, while ART, controlled-released by phase change materials under laser/US stimulation, enhances ROS production via Fe 2+ -mediated decomposition. This triple-enhanced strategy accumulates lipid peroxidation (LPO), significantly improving ferroptosis effects with a tumor suppression rate of 94.3 %. Moreover, ZB enables multimodal imaging and stimulates antitumor immunity, demonstrating its potential as a diagnostic and therapeutic agent. Our findings demonstrate the potential of this ZB@ART system in advancing ferroptosis-based tumor therapies, inspiring future designs of efficient ferroptosis inducers.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xinghao Liu,Nan Li,Xugui Lv,Jingjing Wang,Qingyu Ma,Zheng Xie
Two-dimensional (2D) materials consist of either a single layer or just a few layers of atoms or molecular layers, and their exceptional optoelectronic properties including high carrier mobility, wide spectral absorption range, and optical response from the number of layers. Graphene quantum dots (GQDs) as a small-sized 2D material exhibited unique physical and chemical properties at the quantum scale. In this study, he N, S-doped GQDs (named as Y-GQDs) were synthesized through straightforward solvothermal process using 2,2'-dithiobenzoic acid and o-phenylenediamine as the precursors. The distribution of the prepared GQDs sample was uniform, with height varying between 0.6 and 0.8 nm. The excellent optical properties of Y-GQDs were attributed to the high crystalline graphene structure and rich functional groups including -C-SO 3 -C-, -C-SO 4 -C-, C-N, etc . The optimal excitation and emission wavelengths of Y-GQDs were 380 nm and 535 nm, respectively. Additionally, the multi-color and tunable luminescence characteristics could be achieved by excitation wavelength, solvent, and concentration. Gratifyingly, the N, S-doped GQDs were successfully used to build white light emitting devices via a sol-gel process. The color rendering index reached 83.7 with color temperature of 5306 K, and the GQDs exhibited good optical stability under different driving currents and UV light. This study underscored the significant potential of GQDs in creating promising phosphors for superior lighting applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Hao Ma,Chunyan Huang,Tianqi Tan,Wenting Li,Wei Xu,Yu Shen,Yuhan Li,Ruimei Fang,Fan Dong
Photocatalytic technology is of great significance in environmental purification due to its eco-friendly and cost-effective operations. However, low charge-transfer efficiency restricts the photocatalytic activity of the catalyst. Herein, we report Cs 2 SnBr 6 /C 3 N 4 composite catalysts that exhibit a robust interfacial electron exchange thereby enhancing photocatalytic nitric oxide (NO) oxidation . A comprehensive study has demonstrated the S-scheme electron transfer mechanism. Benefiting from the interfacial internal electric field , the C-Br bond serves as a direct electron transfer channel, resulting in enhanced charge separation. Furthermore, the S-scheme heterojunction effectively traps high redox potential electrons and holes, leading to the production of abundant reactive oxygen radicals that enhance photocatalytic NO abatement. The NO removal rate of the Cs 2 SnBr 6 /C 3 N 4 heterogeneous system can reach 86.8 %, which is approximately 3-fold and 18-fold that of pristine C 3 N 4 and Cs 2 SnBr 6 , respectively. The comprehensive understanding of the electron transfer between heterojunction atomic interfaces will provide a novel perspective on efficient environmental photocatalysis .
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Xu Feiyan,Zhao Feifan,Deng Xianyu,Zhang Jinfeng,Zhang Jianjun,Ai Chenbin,Yu Jiaguo,García Hermenegildo
The rapid increase in atmospheric CO 2 levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO 2 reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO 2 /Bi 2 S 3 heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO 2 -to-CO conversion (14.05 mmol g −1 , 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO 2 into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO 2 conversion systems.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hongwu Liao,Chong Wang,Jiaxian Zheng,Zhuo Chen,Yulin Zhou,Chengning Ye,Xiangfeng Lin,Meng An,Yusuke Yamauchi,Yusuke Asakura,Zhanhui Yuan
Photocatalytic depolymerization of lignin offers a sustainable approach to producing high-value-added aromatic compounds. Recently, carbon nitride has demonstrated notable selectivity for the C C bonds in lignin model compounds. However, limitations of pure carbon nitride include the low mobility of photogenerated electrons and the difficulty in precisely controlling the cleavage pathways and products of C C bonds. In this study, we constructed an S-Scheme heterojunction by in situ loading of Ce ions onto C 3 N 4 to form a CeO 2 /C 3 N 4 composite. This heterojunction achieves efficient lignin depolymerization under blue LED irradiation in an oxygen-rich environment. Comparative analysis indicated that the yield of primary products, benzaldehyde and phenyl formate, increased by 7.8-fold and 7.75-fold, respectively, compared with pure CeO 2 , and by 1.4 and 1.8 times relative to unmodified C 3 N 4 . After optimizing the reaction conditions, dealkalized lignin is applied to the system and successfully depolymerized. Comprehensive characterization and theoretical simulations verify the heterojunction's ability to enhance carrier separation and redox activity, with CeO 2 serving as an active dehydrogenation site that significantly boosts the depolymerization efficiency of lignin model compounds. This photocatalytic strategy presents a valuable step forward in lignin valorization and supports the sustainable utilization of biomass resources.
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