ACS Sustainable Chemistry & Engineering
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2025
·
IF 7.3
Xiongwei Tian,Zheng Chen,Francesco Iacoviello,Mengyin Xie,Wenqing Chu,Yuqun Zhuo
The electroreduction of carbon dioxide (CO2R) presents a promising avenue for mitigating CO2 emissions while producing valuable chemicals. In this work, we report a novel pressure equilibrium strategy tailored for pressurized CO2R in a zero-gap electrolyzer, aiming at accommodating the high-pressure CO2 sources from its capture, utilization, and storage scheme. We investigated the impact of pressure on the CO2R performance under both gaseous and supercritical conditions, while also examining the synergistic interplay of temperature with high pressure. Significant enhancement of energy efficiency (46.5%) with high CO Faradaic efficiency (94.4%) and low cell voltage (−2.72 V) was achieved at 200 mA/cm2 under 75 bar and 80 °C. In addition, we noticed that the agglomeration and migration of salt precipitation within the gas diffusion electrode were effectively suppressed under pressurized conditions, which indicated the potential benefit for prolonged cell stability.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2025
·Vol. 122
·期 18
·e2503292122
·
IF 9.1
Hong Wang,Jiwen Guan,Guangxian Xu,Xavier Mercier,Jinyang Zhang,Haotian Guo,Tongzhu Yu,Huaqiao Gui,Teng Huang,Donald G. Truhlar,Zhandong Wang
Carbonaceous particles are widespread in combustion, atmospheric, extraterrestrial, and nanomaterials environments. Resonance-stabilized radicals (RSRs) are commonly identified in fuel combustion and pyrolysis processes and play an essential role in carbonaceous particle formation. Despite their importance, comprehensive experimental and mechanistic understanding of particle inception through RSR reactions is lacking. This work investigated particle size distribution, chemical composition, and thermal behavior of soot particles generated by the flow reactor pyrolysis reactions of typical RSRs, in particular, 1-indenyl, 1-methylnaphthyl, and 2-methylnaphthyl radicals, and by the pyrolysis of hydrocarbons with a variety of structures. Particle size distributions show soot particles with mobility diameters in an incipient-particle range of 1.3 to 1.6 nm. Laser desorption/ionization mass spectrometry results suggest that soot products consist of much larger covalently bound clusters (CBCs) than those observed in the gas phase. Under our experimental conditions, the CBCs exhibit a phase transition for particles with calculated molecular diameters of around 1.5 nm. Evaporation experiments and thermogravimetric analysis of the soot products reveal distinct thermal characteristics for small and large CBCs. These results implicate CBCs as bridges between gas-phase species and soot particles. The present work provides a soot-inception mechanism called RSR clustering (RSRC) that is characterized by the reactive clustering of RSRs. The RSRC mechanism contrasts with conventional soot formation models that attribute soot inception primarily to the aggregation of large-size polycyclic aromatic hydrocarbons.
研究领域:
燃烧学
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大气化学
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材料科学
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Tianxing Yuan,Xingrong Chen,Yanqin Zhao,Yingqiao Jiang,Bin Li,Ningning Zhao,Jing Zhu,Lei Dai,Ling Wang,Zhangxing He
Vanadium redox flow battery (VRFB), as a potential technology for next-generation energy storage system, is restricted by the slow redox kinetics of vanadium ions. Implementing interface engineering strategies to functionalize the surface of MXene can effectively address this challenge. Herein, a Nb 2 CT x /Nb 2 O 5 Schottky heterostructure is constructed to facilitate high-speed charge transfer at the VRFB electrode through controllable in-situ oxidation. The loading amount of Nb 2 O 5 nanorods on the surface of Nb 2 CT x nanosheets was regulated by varying the hydrothermal reaction time. Density functional theory calculations confirm that the Schottky barrier formed between Nb 2 CT x and Nb 2 O 5 leads to the establishment of an internal electric field and reconfigures the electronic structure of surficial active sites. The rich pore structure of Nb 2 CT x /Nb 2 O 5 electrode effectively shortens the diffusion path for vanadium ions, while its excellent hydrophilicity enhances the interaction between vanadium ions and the electrodes. Compared with graphite felt, Nb 2 CT x /Nb 2 O 5 -2@GF cell shows a 20% increase in energy efficiency (EE) at 150 mA cm −2 cycling, reaching 75%, while maintaining stable performance for over 800 cycles. This means a significant advancement in the development of high-performance electrodes for VRFBs. This work offers an efficient and scalable strategy for the design of redox flow batteries.
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LAB ON A CHIP
·
2025
·
IF 5.4
Xueqing Ren,Xin Wang,Xiaolu Cai,Yi Zou,Peng Chen,Bi-Feng Liu,Yiwei Li
Hydrogel microspheres, derived from natural or synthetic materials, serve as crucial platforms for three-dimensional (3D) cell culture and tissue engineering. While traditional production methods like emulsification and microfluidics are widely used, they often involve complex processes and oil phases that can compromise biocompatibility. Here, we present a novel centrifugal microfluidic device with an air gap for producing hydrogel microspheres. Centrifugal force provides a driving force for uniform parallel channels, enabling high-throughput microsphere generation while ensuring size uniformity. The system enables precise size control through centrifugal speed modulation, producing microspheres with diameters ranging from 140.6 ± 17.3 μm to 417.1 ± 34.4 μm with a coefficient of variation below 4.8%. The air gap within the microchannel establishes a step-structure that enables oil-free microsphere generation while ensuring biocompatibility. Moreover, by blending a collagen solution into sodium alginate as the matrix, oil-free microspheres with an interpenetrating polymer network (IPN) can be fabricated, which exhibit excellent biocompatibility to support the culture and adipogenic differentiation of mesenchymal stem cells (MSCs). When cells are cultured with a microsphere-formed scaffold, they exhibit aggregation behavior for enhanced cell–cell communication, which further elevated their adipogenic differentiation potential. Overall, this simplified, high-throughput approach offers a unique platform for applications in cell delivery, drug screening, and tissue engineering.
研究领域:
微流控
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生物医学工程
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组织工程
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细胞培养
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药物递送
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高分子科学
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干细胞研究
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ADVANCED MATERIALS
·
2024
·
IF 27.4
Chenyang Wang,Wenxuan Yang,Yiran Ding,Pengfei Bai,Ziyue Zeng,Haifeng Lv,Xiang Li,Huiliu Wang,Zhouyang Wang,Mengqi Zeng,Xiaojun Wu,Lei Fu
2D layered materials are regarded as prospective catalyst candidates due to their advantageous atomic exposure ratio. Nevertheless, the predominant population of atoms residing on the basal plane with saturated coordination, exhibit inert behavior, while a mere fraction of atoms located at the periphery display reactivity. Here, a novel approach is reported to attain complete atom activation in 2D layered materials through the construction of an interlayer biatomic pair bridge. The atoms in question have been strategically optimized to achieve a highly favorable state for the adsorption of intermediates. This optimization results from the introduction of new gap states around the Fermi level. Moreover, the presence of the interlayer bridge facilitates the electron transfer across the van der Waals gap, thereby enhancing the reaction kinetics. The hydrogen evolution reaction exhibits an impressive ultrahigh current density of 2000 mA cm −2 at 397 mV, surpassing the pristine MoS 2 by approximately two orders of magnitude (26 mA cm −2 at 397 mV). This study provides new insights for enhancing the efficacy of 2D layered catalysts.
研究领域:
材料科学
·
催化
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纳米技术
·
电化学
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ACS Nano
·
2023
·
IF 17.1
Wenbin Wang,Yun Song,Chengxuan Ke,Yang Li,Yong Liu,Chen Ma,Zongxiao Wu,Junlei Qi,Kai Bao,Lingzhi Wang,Jingkun Wu,Shan Jiang,Jiong Zhao,Chun-Sing Lee,Ye Chen,Guangfu Luo,Qiyuan He,Ruquan Ye
Composition modulation and edge enrichment are established protocols to steer the electronic structures and catalytic activities of two-dimensional (2D) materials. It is believed that a heteroatom enhances the catalytic performance by activating the chemically inert basal plane of 2D crystals. However, the edge and basal plane have inherently different electronic states, and how the dopants affect the edge activity remains ambiguous. Here we provide mechanistic insights into this issue by monitoring the hydrogen evolution reaction (HER) performance of phosphorus-doped MoS2 (P-MoS2) nanosheets via on-chip electrocatalytic microdevices. Upon phosphorus doping, MoS2 nanosheet gets catalytically activated and, more importantly, shows higher HER activity in the edge than the basal plane. In situ transport measurement demonstrates that the improved HER performance of P-MoS2 is derived from intrinsic catalytic activity rather than charge transfer. Density functional theory calculations manifest that the edge sites of P-MoS2 are energetically more favorable for HER. The finding guides the rational design of edge-dominant P-MoS2, reaching a minuscule onset potential of ∼30 mV and Tafel slope of 48 mV/dec that are benchmarked against other activation methods. Our results disclose the hitherto overlooked edge activity of 2D materials induced by heteroatom doping that will provide perspectives for preparing next-generation 2D catalysts.
研究领域:
材料科学
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催化化学
·
理论计算
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ACS Nano
·
2022
·
IF 18.027
Yongping Dai,Qiang Yu,Xiaoxin Yang,Kun Guo,Yan Zhang,Yushuang Zhang,Junrong Zhang,Jie Li,Jie Chen,Haiqin Deng,Tianhao Xian,Xiao Wang,Jian Wu,Kai Zhang
Ultrafast photonics has become an interdisciplinary topic of great consequence due to the spectacular progress of compact and efficient ultrafast pulse generation. Wide spectrum bandwidth is the key element for ultrafast pulse generation due to the Fourier transform limitation. Herein, monoclinic Nb2GeTe4, an emerging class of ternary narrow-gap semiconductors, was used as a real saturable absorber (SA), which manifests superior wide-range optical absorption. The crystallization form and growth mechanism of Nb2GeTe4 were revealed by a thermodynamic phase diagram. Furthermore, the Nb2GeTe4–SA showed reliable saturation intensity and larger modulation depth, ascribed to a built-in electric field driven by the asymmetric crystal architecture confirmed via X-ray diffraction, polarized Raman spectra, and scanning transmission electron microscopy. Based on the Nb2GeTe4–SA, femtosecond mode-locked operation with good overall performance was achieved by a properly designed ring cavity. These results suggest that Nb2GeTe4 shows great promise for ultrafast photonic applications and arouse interests in exploring the intriguing properties of the ternary van der Waals material family.
研究领域:
材料科学
·
光学工程
·
物理学
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Results in Physics
·
2024
·
IF 4.4
Fazal Kabir,Adil Murtaza,Wasif ur Rehman,Awais Ghani,Sen Yang
Diluted magnetic semiconducting nanostructures are attractive materials for spintronics applications. This study focuses on the fabrication of (Gd, Fe) co-doped ZnO nanoparticles (NPs). X-ray diffractogram analysis confirms a monophase hexagonal wurtzite structure, matching JCPDS file number (36–1451). The Scherrer equation and Williamson-Hall plot are used to measure crystal size and strain, respectively. Scanning electron microscopy reveals a spherical surface morphology, and energy-dispersive X-ray analysis confirms elemental composition. Transmission electron microscopy shows average diameter of 17–52 nm and fringe spaces of 0.269–0.245 nm. The incorporation of dopant ions leads to a slight reduction in the bandgap. The Fe3+ and Gd3+ oxidation states of the dopant elements are confirmed using X-ray photoelectron spectroscopy. Functional groups are identified via Fourier transform spectroscopy, and structural defects are identified by photoluminescence analysis. Pristine ZnO NPs exhibit diamagnetic behavior, while the doped samples demonstrate ferromagnetic properties. The observed ferromagnetism in the doped NPs is attributed to bound magnetic polaron interactions. Electron paramagnetic resonance spectroscopy detects unpaired electrons in samples, with g factor values of approximately 2. The co-doping of Gd and Fe presents a promising approach for achieving ferromagnetism in ZnO systems, offering significant potential for advancement in spintronics technology.
研究领域:
材料科学
·
物理学
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Carbon Energy
·
2024
·Vol. 6
·期 9
·e535
·
IF 19.5
Zhimin Niu,Yan Gao,Tianhui Wu,Fei Zhang,Ran Zhao,Zijia Chen,Yiming Yuan,Tifeng Jiao,Jianmin Gu,Li Lu,Desong Wang
Rechargeable neutral aqueous zinc−air batteries (ZABs) are a promising type of energy storage device with longer operating life and less corrosiveness compared with conventional alkaline ZABs. However, the neutral ZABs normally possess poor oxygen evolution reactions (OERs) and oxygen reduction reactions performance, resulting in a large charge–discharge voltage gap and low round-trip efficiency. Herein, we demonstrate a sunlight-assisted strategy for achieving an ultralow voltage gap of 0.05 V in neutral ZABs by using the FeOOH-decorated BiVO 4 (Fe-BiVO 4 ) as an oxygen catalyst. Under sunlight, the electrons move from the valence band (VB) of Fe-BiVO 4 to the conduction band producing holes in VB to promote the OER process and hence reduce the overpotential. Meanwhile, the photopotential generated by the Fe-BiVO 4 compensates a part of the charging potential of neutral ZABs. Accordingly, the energy loss of the battery could be compensated via solar energy, leading to a record-low gap of 0.05 V between the charge and discharge voltage with a high round-trip efficiency of 94%. This work offers a simple but efficient pathway for solar-energy utilization in storage devices, further guiding the design of high energy efficiency of neutral aqueous ZABs.
研究领域:
材料科学
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能源存储技术
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电化学
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Analytical Methods
·
2020
·Vol. 12
·期 26
·3361-3367
·
IF 2.596
Wenshuai Li,Guorui Wu,Min Wang,Aiqin Yue,Weijun Du,Dingbin Liu,Jinzhong Zhao
Class A saponins are responsible for the taste of soybean products, and the rapid identification of class A saponins from soybean food is essential for both food safety and cultivar screening. In this study, we propose a colorimetric assay based on the coupling of gap ligase chain reaction (Gap-LCR) with DNAzyme to detect the target GmSg-1 genes of class A soybean saponins with the naked eye, without the involvement of expensive instruments. The limits of detection (LODs) for the GmSg-1a and GmSg-1b genes were determined to be 0.1618 and 0.1625 μM, respectively, with a linear range of 0.2–1.2 μM. The DNAzyme-based Gap LCR assay was successfully employed to identify the target genes from different soybean cultivars, providing a simple means for monitoring the quality of soybean products.
研究领域:
食品科学
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分子生物学
·
分析化学
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高影响因子
IEEE TRANSACTIONS ON INSTRUMENTATION AND MEASUREMENT
·
2026
·
IF 7
Zhen Gui,Luheng Wang,Lijuan Lan,Dingyu Guo
High-precision real-time monitoring of gaps and pressure is essential in precision manufacturing and robotic manipulation. This study develops a transducer system based on a coil-shaped sensor made of carbon nanotube-filled silicone rubber composite material, capable of dual-mode detection of both gap and pressure. The system is supported by custom-developed hardware circuitry and host computer software. A critical impedance threshold is employed to distinguish between non-contact and contact processes, while the impedance change rate is used to differentiate loading and relaxation stages. The non-contact gap is determined using the impedance angle–gap relationship due to its higher sensitivity. The loading pressure is estimated through impedance magnitude–pressure calibration; during relaxation, the pressure is inversely interpolated using the magnitude–pressure relationships of adjacent calibration points (0.1/0.2/0.3/0.4 MPa). Experimental results indicate maximum errors of 3.0 % F.S. for gap measurement and 8.0 % F.S. for pressure measurement. This study lays a preliminary foundation for industrial applications in long-term gap/pressure monitoring.
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JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Ran Wang,Yawei Wang,Shufang Chang,Shu Jin,Yinlin Shao,Xiaoxiang Xu
Complete solid solutions between LaTaON 2 and SrZrO 3 , i.e. (LaTaON 2 ) 1−x (SrZrO 3 ) x (0 ≤ x ≤ 1) have been built which are very useful in tailoring many important parameters of LaTaON 2 . Band gap of LaTaON 2 becomes tunable by controlling the level of solid solutions with SrZrO 3 . Structural distortions, defects (e.g. Ta 4+ species) concentration and surface hydrophilicity of LaTaON 2 are largely improved by introducing SrZrO 3 in the structure. These modifications contribute to much enhanced photocatalytic activities of solid solutions for oxygen production which clearly outperform pristine LaTaON 2 under visible light illumination. Apparent quantum efficiency as high as 0.87% at 420 ± 20 nm was achieved at (LaTaON 2 ) 0.6 (SrZrO 3 ) 0.4 (x = 0.4). Further analysis suggest that introducing SrZrO 3 results in realignment of band edge positions of LaTaON 2 so as to be more appropriate for water splitting reactions.
研究领域:
材料科学
·
光催化化学
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危险品化学品经营许可证（带存储）