Nature Communications
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2024
·Vol. 15
·期 1
·1-9
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IF 14.7
Shen Jiafu,Huang Xi,Dai Yu,Zhang Xiaojin,Xia Fan
Low-grade heat is abundant and ubiquitous, but it is generally discarded due to the lack of cost-effective recovery technologies. Ion thermoelectric cells are an affordable and straightforward approach of converting low-grade heat into usable electricity for sustainable power. Despite their potential, ion thermoelectric cells face challenges such as limited Seebeck coefficient and required series integration. Here, we demonstrate that the N-type and P-type conversion of ion thermoelectric cells can be achieved through the phase transition of temperature-sensitive hydrogel containing the triiodide/iodide redox couple. Through the strong interaction between the hydrophobic region of the hydrogel and triiodide, the hydrophobic side selectively captures triiodide and the hydrophilic side repels triiodide, raising the concentration difference of triiodide and thereby increasing the Seebeck coefficient. Specifically, the Seebeck coefficient of the N-type ion thermoelectric cells is 7.7 mV K −1 , and the Seebeck coefficient of P-type ion thermoelectric cells is −6.3 mV K −1 (Δ T = 15 K). By connecting 10 pairs of the N-type and P-type ion thermoelectric cells, we achieve a voltage of 1.8 V and an output power of 85 μW, surpassing the reported triiodide/iodide-based ion thermoelectric cells. Our work proposes a phase transition strategy for the N-P conversion of ion thermoelectric cells, and highlights the prospect of series integrated hydrogel ion thermoelectric cells for low-grade heat harvesting.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Yujie Cheng,Binbin Wang,Yueyue Lv,Xiaokang Zhang,Yue Han,Yaowu Wang,Shilong He,Yao Li,Lingwei Xue
The electron transport layer (ETL) is a major component of inverted perovskite solar cells (PSCs). It is an effective method for preparing efficient and stable organic ETLs to solve problems such as poor interface contact, adverse energy-level matching, and the lack of a significant passivation effect on perovskites. In this work, two structurally similar n-type branched shoulder-chain small molecules, CY3 and CY4, incorporating [6,6]-phenyl C61-butyric acid methyl ester (PCBM), were established as ETLs for inverted PSCs. The results of experimental tests showed that CY3 and CY4 could effectively passivate electron vacancy defects in perovskites, optimize the energy level alignment between the layers of the PSCs, and significantly improve the interface contact between the ETL and the perovskite layer. Consequently, the PSCs with PCBM:CY4 as the ETL achieved a high power conversion efficiency (PCE) of 19.80% and a stability of 760 h in an air atmosphere, compared to PCBM:CY3 (18.78%, 620 h). Our results provide theoretical guidance and a foundation for constructing high-performance ETLs.
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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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ELECTROCHIMICA ACTA
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2024
·
IF 5.5
Lei Zhang,Bing Sun,Qinghua Liu,Lin Song,Teibang Zhang,Xiaobo Duan
Extensive research has focused on the lithium (Li) metal anode, but progress in developing this technology has been hindered by the formation of lithium dendrites and their irreversible effects. In this study, an inorganic LiF-Li 3 N-rich solid electrolyte interface (SEI) is established in ether electrolyte through the direct use of 2,3-difluoro-5-(trifluoromethyl)pyridine (DP) to enable uniform Li deposition and enhance interfacial properties for a stable Li metal anode. Theoretical calculations show that DP has a higher tendency to decompose on lithium metal. An alternative approach involving the inclusion of additional anions into the solvation sheath of Li + ions using weakly solvating solvents is proposed. During Li plating, DP is reduced to form a LiF and Li 3 N-rich SEI, resulting in a heterogeneous SEI layer on the Li metal anode surface. This approach allows stable cycling of Li|Li cells for over 1800 h at current densities of 5 mA cm −2 and 15 mAh cm −2 . The method presented here has potential significance in the identification of suitable electrolytes for future research on lithium metal anodes.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yueer Ma,Zhao Zhang,Wei Chen,Qianlin Zhang,Shuai Chang,Mei Pan,Xingqiang Lv,Hui Chang
A novel synthetic strategy is proposed to create high zero-valent platinum (Pt) components, sub-nanometer Pt clusters, and three-dimensional (3D) Pt/ nitrogen-doped MXene (N-Ti 3 C 2 T x ) catalyst through electrostatic self-assembly combined with non-in-situ doping pyrolysis. Compared with the primary Pt/Ti 3 C 2 T x , the N-doped Pt/N-Ti 3 C 2 T x , which has a 3D wrinkled porous structure, increases the residence time of methylcyclohexane (MCH) on the catalyst surface during gas–solid reactions and improves the mass transfer efficiency of MCH. In addition, the N-doped Pt/N-Ti 3 C 2 T x , which optimizes the electronic coordination environment, produces sub-nanometer Pt clusters, in which Pt mainly exists as Pt (0) (80.78 %) and avoids the presence of low catalytic activity Pt (IV). The Pt 0.5% /N-MXene catalyst exhibits significant catalytic performance in the dehydrogenation of MCH in a fixed-bed reactor, with a hydrogen evolution rate of 636.30 mmol·g Pt -1 ·min - 1 , which significantly surpasses 176.60 mmol·g Pt -1 ·min - 1 for N-undoped Pt 1% /MXene and 78.13 mmol·g Pt -1 ·min - 1 for commercial Pt 1% /TiO 2 . Density functional theory calculations, Pt/N-Ti 3 C 2 T x exhibits lower Pt electronic states and has a d -band center closer to the Fermi level than Pt/Ti 3 C 2 T x . This configuration leads to the stronger MCH adsorption on the Pt sites of Pt/N-Ti 3 C 2 T x , promoting faster H 2 generation and release, thereby achieving a higher catalytic activity.
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ACS Catalysis
·
2025
·
IF 13.1
Qianqian Song,Yingbing Zhang,Ziyang Wu,Min Kuang,Jun Chen,Jianping Yang
The electrocatalytic urea synthesis has emerged as a promising alternative strategy to replace the current energy-intensive industrial Haber–Bosch processes which are limited by sluggish C–N coupling and low selectivity because of the unmatched reduction kinetics of CO2 and nitrogen-based precursors. Herein, a thermodynamically spontaneous early stage C–N coupling pathway of *CO2 + *NO → *NOCO2 is established through the asymmetric bridging-adsorption of CO2 enabled by hydroxycarbonate-induced CO32–-Cu2+ dual sites on the tandem electrocatalyst of copper carbonate hydroxide and iron oxide grown on carbon fibers (CuCH/α-Fe2O3–CFs). This asymmetric adsorption induces a pronounced electron-deficient state of carbon atoms in CO2 due to bidirectional electron transfer toward both the CO32– and the Cu2+ centers. Coupled with the directional migration of *NO intermediates at the interface, effectively suppress the subsequent protonation of *CO2 while promoting nucleophilic attack by *NO, thereby driving spontaneous initial C–N coupling of *CO2 and *NO and significantly lowering the energy barrier of the C–N coupling step. The results demonstrate a urea Faradaic efficiency of 78.7% and urea yield rate of 1794.6 μg h–1 mgcat–1 at an ultralow applied potential of −0.20 V vs RHE, surpassing most reported catalysts to date.
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CHINESE JOURNAL OF CHEMISTRY
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2024
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IF 5.5
Dongxiao Wang,Zheng Lan,Yue Li,Ying Huang,Kun Yin,Lixia Yang,Liangjiu Bai,Donglei Wei,Huawei Yang,Hou Chen,Mingchuan Luo
Comprehensive Summary Photocatalytic aerobic oxidative desulfurization (PAODS) is a sustainable alternative technology to traditional, energy-intensive fuel desulfurization methods. Nonetheless, its advancement is hindered by the notable challenge of inadequate electron-hole separation efficiency within the existing catalytic systems. Herein, a Janus 2D/2D heterostructure composed of Co 3 O 4 and CoMoO 4 is reported for the PAODS of thiophenic sulfides. Through a combination of detailed experimental characterizations and density functional theory (DFT) calculations, we elucidate the formation of a type II p-n heterojunction in the catalyst, significantly enhancing electron-hole separation through electric field force and reducing the possibility of electron-hole recombination due to the spatial separation of redox centres. The photocatalyst exhibits exceptional activity and demonstrates an impressive performance of 10.4 mmol·g –1 ·h –1 in the oxidation of dibenzothiophene (DBT). Moreover, the photocatalyst demonstrates profound desulfurization capabilities in real diesel, reinforcing its promising prospects for industrial application. These discoveries provide invaluable insights, both scientifically and practically, towards the development of advanced photocatalysts for PAODS processes.
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Molecular Catalysis
·
2025
·
IF 4.9
Bo Jiang,Shu-Lin Liu,Zhe-Yan Jin,Zhao Wang,Bin-Can Cheng,Ze-Long Guan,Ying Hong,Zhao Wei,Zhi Qiao,Jian Tao,Bao-Lian Su
Selective hydrogenation driven by heat is a critical industrial process for purifying alkene feedstocks with serious problems of energy and H 2 consumption. Photochemistry-assisted strategy offers a sustainable alternative owing to its superiority of H 2 -free reaction under ambient temperature, unfortunately, with a challenging demand on efficient catalysts. Herein, a wide-spectrum-responsive Pd/N-TiO 2 photo-thermal catalyst was developed by a solvothermal method for photochemistry-assisted selective hydrogenation of butadiene in propene. It shows an excellent catalytic performance, with 100 % alkenes selectivity and 100 % butadiene conversion under irradiation of full-light (i.e., 320 nm∼780 nm). Notably, over 53 % butadiene conversion with 100 % alkenes selectivity was successfully retained on Pd/N-TiO 2 after shortening the wavelength range to visible light, much superior to that on Pd-TiO 2 (i.e., <1 % butadiene conversion). Further exploration reveals that the nitrogen doping extends the light-responsive wavelength of titanium oxide from ∼380 nm to above 500 nm owing to the formation of Ti 3+ and oxygen vacancies, which later create a defect energy level (i.e., ∼-0.53 to -0.12 eV) between the valence-conduction band of TiO 2 . The wide spectral response of N-TiO 2 enhances the water photolysis to produce intermediate hydrogen ([H]) that acts as the hydrogen source for the tandem butadiene hydrogenation over the Pd surface. The work indicates that developing a dual-functional catalyst with an expanded light-responsive wavelength is an efficient way to enhance the photochemistry-assisted selective hydrogenation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yongjie Jiang,Anqi Li,Qichang Pan,Shunchao Wang,Man Zhang,Sijiang Hu,Yahao Li,Hongqiang Wang,Qingyu Li,Fenghua Zheng
Iron sulfides have shown great potential as anode materials for sodium-ion batteries (SIBs) because of their high sodium storage capacity and low cost. Nevertheless, iron sulfides generally exhibit unsatisfied electrochemical performance induced by sluggish electron/ion transfer and severe pulverization upon the sodiation/desodiation process. Herein, we constructed a yolk-shell FeS@NC nanosphere with an N-doped carbon shell and FeS particle core via a simple hydrothermal method, followed by in-situ polymerization and vulcanization. The FeS particles intimately coupled with N-doped carbon can accelerate the electron transfer, avoid severe volume expansion, and maintain structural stability upon repeated sodiation/desodiation process. Furthermore, the small particle size of FeS can shorten ion-diffusion distance and facilitate ion transportation. Therefore, the FeS@NC nanosphere shows excellent cycling performance and superior rate capability that it can deliver a high capacity of 520.1 mAh g −1 over 800 cycles at 2.0 A g −1 and a remarkable capacity of 625.9 mAh g −1 at 10.0 A g −1 .
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Nano Materials Science
·
2025
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IF 17.9
Yang He,Qingling Ruan,Han Kang,Ling Ye,Ya-Xiong Wang,Tiefeng Liu,Hairong Cheng,Xingxing Gu
Li-S batteries (LSBs), with their exceptional theoretical energy density, are widely recognized as a leading option for future energy storage solutions. Nevertheless, on the way to commercialization, the poor conductivity of the positive electrode, the easy dissolution loss of the active substance, and the serious dendrite growth of the negative electrode are stumbling blocks. Therefore, this work designs a novel tungsten and nitrogen-co-doped nanoporous carbon (W,N-C) with multifunction: chemically adsorbs the polysulfides to inhibit shuttling behavior, accelerates Li + transfer, and catalyzes polysulfides redox to address the aforementioned issues of LSBs. As expected at the beginning of the design, the prepared W,N-C-5/S composites cathodes demonstrate excellent performances, i.e., delivering an initial capacity of 944.9 mAh g −1 and a reversible capacity of 771.7 mAh g −1 after 500 cycles at 1 C, significantly outperforming the N-C/S contrast sample. The proposed method offers a feasible solution for boosting the electrochemical performance of LSBs.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Xiaoshun Wei,Xuechun Yang,Yun Guo,Yinzhong Liu,Lingchao Wang,Qingjie Wang,Lingli Cheng,Zheng Jiao
In this study, a novel UV-enhanced Mg-doped MOF-ZnO sensor was investigated for its efficient detection of n-butanol gas at lower temperatures. The composite samples were prepared by the co-precipitation method with the appropriate component ratio. The structure, morphology, and optical properties of the as-prepared samples were systematically analyzed through XRD, SEM, TEM, BET, XPS, and UV–vis characterizations. The gas-sensitive performances based on the pristine MOF-ZnO and Mg-doped MOF-ZnO sensor series with the doping levels of 1 %, 3 %, 5 %, and 7 % (wt%) were comprehensively evaluated by adopting the gas-sensitive system. Among them, the 3 % Mg:MOF-ZnO sensor has given prominence to the largest specific surface area and highest oxygen vacancy concentration demonstrating the most excellent gas-sensing performance. Furthermore, with the aid of UV excitation, the 3 % Mg:MOF-ZnO sensor had achieved the enhanced response value of 2049 that was 4.44 times higher than that of pristine MOF-ZnO to 100 of ppm n-butanol at a low temperature of 246 °C, additionally presented out the superior reproducibility with speedy response/recovery time (12/22 s), the theoretical detection limit as low as 200 ppb, as well as the excellent long-term stability and selectivity for n-butanol. This study offers a promising strategy for the well-development of high-performance n-butanol sensors.
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JOURNAL OF MEDICINAL CHEMISTRY
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2024
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IF 6.8
Yi Huang,Fengling Liu,Shuhua Ren,Yuanqing Ding,Man Chi,Weiwei Huang,Wenjing Gu,Hewen Qian,Yaxia Yuan,Shurong Hou,Xiabin Chen,Lei Ma
Idiopathic pulmonary fibrosis (IPF) is a progressive and lethal lung disease with an elusive etiology. Aberrant activation of c-Jun N-terminal kinase 1 (JNK1) has been implicated in its pathogenesis. Through a combination of structure-based drug design and structure–activity relationship (SAR) optimization, a series of pyrimidine-2,4-diamine scaffold derivatives have been developed as potent JNK1 inhibitors. Compound E1 was identified with low nanomolar JNK1 inhibitory potency (IC50 = 2.7 nM). The introduction of a dimethylamine side chain has significantly enhanced the ability of E1 to inhibit c-Jun phosphorylation, surpassing the clinical candidate CC-90001. Molecular dynamics simulations revealed a binding free energy of −50.46 kcal/mol for E1. Moreover, E1 displayed satisfactory pharmacokinetic properties, with a bioavailability of 69% in rats. Furthermore, compound E1 exerted significant antifibrotic effects in a bleomycin-induced IPF mouse model and prevented a TGF-β-induced epithelial-to-mesenchymal transition in vitro. These findings position E1 as a promising lead for further drug development targeting IPF.
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