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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Enhanced electrocatalytic activity of 2D ordered mesoporous nitrogen-rich carbon nanosheets functional NiFe2O4 nanospheres for ultrasensitive detection of chlorogenic acid in natural samples

Yaqi Yang,Pu Wang,Zhiwang Luo,Jiejun Li,Yilin Wang,Zhen Li,Chao Chen,Yixi Xie,Pengcheng Zhao,Junjie Fei

Two-dimensional (2D) porous carbon nanosheets loaded with bimetallic oxide nanospheres are expected to be very attractive electrocatalysts. In this work, we constructed ordered mesoporous nitrogen-rich carbon on the surface of ultrathin-reduced graphene oxide (rGO) using the self-assembly of block polymers and compared the effect of pore structure on the sensing performance. The rGO wrapped by N-doped ordered porous carbon possesses a large specific surface area of 784.9 m 2 /g. The composite with NiFe 2 O 4 nanospheres with rough surfaces effectively prevented the interlayer accumulation of mNPC@rGO. Meanwhile, the multivalent form of metal elements in NiFe 2 O 4 facilitates the redox reaction. These distinct advantages combine to create an active surface that strongly binds to chlorogenic acid molecules (CGA). Importantly, we have computationally analyzed the reaction mechanism of mNPC@rGO/NiFe 2 O 4 electrocatalytic CGA molecules by density functional theory. In the best case, the mNPC@rGO/NiFe 2 O 4 /GCE sensor has a limit of detection (LOD) as low as 2 × 10 −11 M and a wide linear range (1 × 10 −10 −2 × 10 −5 M). The sensor displays a remarkable level of selective response to CGA in the presence of other co-interfering species. Furthermore, it has superb repeatability and reproducibility for CGA. The sensor has shown outstanding recovery (95.9%−104.9%) in the practical viability of detecting CGA in food, natural products, and biological samples. This work not only provides a new candidate for the accurate detection of CGA, but also provides insight into the exploration of advanced sensing materials.

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Applied Materials Today · 2023 · IF 8.3

NIR-responsive GO/Ag2S heterostructure for rapid bacteria-killing and wound healing

Jingwen Wu,Tian Deng,Qian Wu,Yun Qiu,Yan Wei,Qin Zhao,Yufeng Zhang

Many efforts have been made to treat infections; however, it is difficult to treat bacterial infections effectively with a single antibacterial strategy. Therefore, it is imperative to develop drugs or materials with multiple synergistic mechanisms. Graphene oxide/silver sulfide (GO/Ag 2 S) heterostructure would become potential nano-antibiotics that display a synergistic photothermal/photodynamic antibacterial mechanism. The material was characterized with different tests, meanwhile, density functional theory (DFT), electrochemical tests, and electron paramagnetic resonance (EPR) were also tested. The heterostructure nanosheets showed significant therapy via effective photothermal/photodynamic conversion and displayed antibacterial activity against both gram-positive S. aureus and gram-negative E. coli . In addition, we found that GO/Ag 2 S heterostructure could disrupt the integrity of bacterial membranes and inhibit the growth of bacteria. We confirmed its antibacterial effects in subcutaneous abscess models as well. Therefore, GO/Ag 2 S heterostructure could be a viable alternative option for antibiotic development.

CAS / MDL: 7782-42-5
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Food Analytical Methods · 2023 ·Vol. 16 ·期 6 ·1131-1144 · IF 2.9

Covalent Organic Framework/Reduced Graphene Oxide Composite for Solid-Phase Microextraction of Polycyclic Aromatic Hydrocarbons in Honey

Yu Chen,Luo Xiaogang,Wu Fengshou,Zhang Juan

A covalent organic framework/reduced graphene oxide composite (COF/rGO) was fabricated by facile ultrasonic self-assembly strategy and further coated onto stainless-steel wire by physically adhesion for headspace solid-phase microextraction (HS-SPME) of polycyclic aromatic hydrocarbons (PAHs) prior to their determination by gas chromatography-flame ionization detection (GC-FID). Compared with the individual porphyrin-based COF and GO, the as-prepared COF/rGO composite effectively prevented the stacking of GO nanosheets and exhibited enhanced extraction efficiency due to the synergistic effect, with the enrichment factor up to 8816 for phenanthrene. The morphology, structure, and stability of COF/rGO composite was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, thermogravimetric analysis, and N 2 adsorption–desorption. Effective adsorption and desorption parameters including extraction temperature, extraction time, desorption temperature, desorption time, agitation speed, and ionic strength were optimized. The established HS-SPME/GC-FID method based on COF/rGO composite fiber was evaluated in terms of linear ranges from 0.5 to 250.0 ng mL −1 with R 2  ≥ 0.9985, limits of detection in the range of 0.09–0.59 ng mL −1 , and limits of quantitation in the range of 0.31–1.97 ng mL −1 . The intra-day, inter-day, and fiber-to-fiber relative standard deviations (RSDs) were in the range of 1.86–4.37%, 2.48–5.40%, and 3.51–7.81%, respectively. The established method was employed to determine trace level of PAHs in honey with good recoveries (62.99–128.8%) and reliable reproducibility (0.51–7.63%).

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Nanoscale · 2023 ·Vol. 15 ·期 37 ·15318-15327 · IF 6.7

Scalable fabrication of ultra-fine lithiophilic nanoparticles encapsulated in soft buffered hosts for long-life anode-free Li2S-based cells

Bo Zhou,Ting Li,Anjun Hu,Baihai Li,Runjing Li,Chuan Zhao,Nian Chen,Miao He,Jing Liu,Jianping Long

Minimizing the amount of metallic lithium (Li) to zero excess to achieve an anode-free configuration can help achieve safer, higher energy density, and more economical Li metal batteries. Nevertheless, removal of excess Li creates challenges for long-term cycling performance in Li metal batteries due to the lithiophobic copper foils as anodic current collectors. Here, we improve the long-term cycling performance of anode-free Li metal batteries by modifying the anode-free configuration. Specifically, a lithiophilic Au nanoparticle-anchored reduced graphene oxide (Au/rGO) film is used as an anodic modifier to reduce the Li nucleation overpotential and inhibit dendrite growth by forming a lithiophilic LixAu alloy and solid solution, which is convincingly evidenced by density functional theory calculations and experimentally. Meanwhile, the flexible rGO film can also act as a buffer layer to endure the volume expansion during repeated Li plating/stripping processes. In addition, the Au/rGO film promotes a homogeneous distribution of the electric field over the entire anodic surface, thus ensuring a uniform deposition of Li during the electrodeposition process, which is convincingly evidenced by finite element simulations. As expected, the Li||Au/rGO-Li half-cell shows a highly stable long-term cycling performance for at least 500 cycles at 0.5 mA cm−2 and 0.5 mA h cm−2. A Li2S-based anode-free full cell allows achieving a stable operation life of up to 200 cycles with a capacity retention of 63.3%. This work provides a simple and scalable fabrication method to achieve anode-free Li2S-based cells with high anodic interface stability and a long lifetime.

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Nanoscale Advances · 2023 ·Vol. 5 ·期 18 ·4852-4862 · IF 4.7

High-performance flower-like and biocompatible nickel-coated Fe3O4@SiO2 magnetic nanoparticles decorated on a graphene electrocatalyst for the oxygen evolution reaction

Li Ye,Pengcheng Zhu,Tianxing Wang,Xiaolei Li,Lin Zhuang

The electrocatalytic oxygen evolution reaction (OER) plays a crucial role in renewable clean energy conversion technologies and has developed into an important direction in the field of advanced energy, becoming the focus of basic research and industrial development. Herein, we report the synthesis and application of flower-like nickel-coated Fe3O4@SiO2 magnetic nanoparticles decorated on a graphene electrocatalyst for the OER that exhibit high efficiency and robust durability. The catalysts were optimized using a rotating ring-disk electrode to test their oxygen evolution properties in 1.0 M KOH solution. Importantly, owing to the high specific surface area and conductivity of C3N4 and graphene, the as-synthesized Fe3O4@SiO2@NiO/graphene/C3N4 exhibits a small Tafel slope of 40.46 mV dec−1, low overpotential of 288 mV at 10 mA cm−2, and robust OER durability within a prolonged test period of 100 h. The cytotoxicity of Fe3O4@SiO2, Fe3O4@SiO2@NiO, and Fe3O4@SiO2@NiO/graphene/C3N4 was evaluated in HeLa and MC3T3-E1 cells, demonstrating that they are efficient and biocompatible catalysts for the OER. Owing to its excellent electrocatalytic efficiency and eco-friendliness, Fe3O4@SiO2@NiO/graphene/C3N4 has considerable potential as a new multifunctional composite for large-scale applications in catalysis, biology, medicine, and high-efficiency hydrogen production.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Exploring Lipoic Acid-Mediated Dynamic Bottlebrush Elastomers as a New Platform for the Design of High-Performance Thermally Conductive Materials

Sijia Zheng,Haiyan Xue,Jun Yao,Yang Chen,Michael A. Brook,Muhammad Ebad Noman,Zhihai Cao

The development of high-performance thermally conductive interface materials is the key to unlocking the serious bottleneck of modern microelectronic technology through enhanced heat dispersion. Existing methods that utilize silicone composites rely either on loading large doses of randomly distributed thermal conductive fillers or on filling prealigned thermal conductive scaffolds with liquid silicone precursors. Both approaches suffer from several limitations in terms of physical traits and processability. We describe an alternative approach in which malleable silicone matrices, based on the dynamic cyclic disulfide nature cross-linker (α-lipoic acid), are readily prepared using ring-opening polymerization. The mechanical properties of the resultant dynamic silicone matrix are readily tunable. Stress-dependent depolymerization of the disulfide network demonstrates the ability to reprocess the silicone elastomer matrix, which allows for the fabrication of highly efficient thermal conductive composites with a 3D interconnecting, thermally conductive network (3D-graphite/MxBy composites) via in situ methods. Applications of the composites as thermal dispersion interface materials are demonstrated by LEDs and CPUs, suggesting great potential in advanced electronics.

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LANGMUIR · 2023 · IF 3.9

Synergy of Two Intermolecular Hydrogen Bonds Promotes Highly Sensitive and Selective Room-Temperature Dimethyl Methylphosphonate Sensing: A Case of rGO-Based Gas Sensors

Zhimin Yang,Zefeng Wei,Yunpeng Xing,Liang Zhao,Yaqing Zhang,Congcong Xin,Teng Fei,Sen Liu,Tong Zhang

The development of room-temperature chemiresistive gas sensors with low limit of detection, high sensitivity, and selectivity for dimethyl methylphosphonate (DMMP) detection remains a challenge. Herein, a synergy of the two intermolecular hydrogen bond-promoted approach was proposed to fabricate a room-temperature DMMP sensor with enhanced performances. As a proof of concept, ternary p-hexafluoroisopropanol phenyl (HFIP) functionalized polypyrrole-reduced graphene oxide hybrids (HFIP-PPy-rGO) were rationally designed. During the sensing process, rGO serves as a conductive carrier, ensuring that the sensors operate at room temperature, and both HFIP and PPy act as adsorption sites for DMMP through hydrogen bonding interactions. As expected, the HFIP-PPy-rGO sensor exhibits high selectivity and sensitivity to DMMP. Besides, the HFIP-PPy-rGO sensor also possesses excellent linear response to DMMP and long-term stability. Experimental results and quartz crystal microbalance measurements prove that the specific recognition of DMMP is realized by forming two intermolecular hydrogen bonds between HFIP and DMMP, as well as PPy and DMMP. Additionally, the introduction of HFIP groups also contributes to adjusting device conductivity, enhancing signal conversion function. To put the DMMP sensor into potential practical application, the obvious sensing response to different DMMP concentrations in soil was confirmed, and a wireless detection system was built to realize real-time monitoring of DMMP concentrations in the surroundings. Overall, this study provides a facile and practical solution for improving the sensing performance of room-temperature sensors based on the hydrogen bond theory.

CAS / MDL: 7782-42-5 110-46-3
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CHEMICAL PAPERS · 2023 ·Vol. 77 ·期 11 ·6637-6646 · IF 2.2

The comparing on the adsorption/desorption of Pd(II) and Pt(IV) ions by using 4-chlorophenyl sulfoxide modified the reduced graphene oxide composite

Chen Lei,Li Rongxin,Li Yuanlong,Shu Qijiang,Yang Tao

The reduced graphene oxide aerogel modified by 4-chlorophenyl sulfoxide was obtained by a simple self-assemble process under the basic reduction-oxide condition, then freeze-dried for future using. The prepared aerogel was shortly named 4CS-rGO, which was characterized by Fourier transform infrared spectroscopy, Raman spectroscopy, scanning electron microscope, et al. 1 mg of 4CS-rGO composite was used as an adsorbent to adsorb Pd(II) and Pt(IV) in 1.0 mL 40 mM Britton-Robinson buffer solution with various pH. The adsorption efficiency of Pd(II) increased with the increase in pH, whereas the hydrolysis of Pd(II) happened at pH 13, and the maximum adsorption efficiency of Pd(II) was 91.82% at pH 12, which was mainly driven by electrostatic attraction. Besides, the adsorption behavior of the 4CS-rGO composite for Pt(IV) was explored to evaluate the possibility to isolate Pd(II) and Pt(IV) ions by using aerogel. We found that, quite interestingly, hydrogen bond, hydrophobic interaction and van der Waals force can strongly conquer electrostatic repulsion driven Pt(IV) ions adsorption behavior at pH 5, and Pt(IV) ions displaced by cationic surfactant. Moreover, a tighter Pt(IV) ions adsorption behavior than Pd(II) ions was observed while we adsorb them respectively with/without 4-chlorophenyl sulfoxide modified the graphene, while branched TBAB was easier and more effectively replaced the adsorbed Pt(IV) ions than strained CTAB.

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TRIBOLOGY INTERNATIONAL · 2023 · IF 6.2

Improving the tribological properties of ZrO2(Y2O3)-graphite composites at high temperature through three-dimensional continuous structure

Pengyu Lin,Junjie Song,Xin You,Qiuan Sun,Tao Li,Jiaxin Si,Haifeng Wang,Litian Hu,Yongsheng Zhang

ZrO 2 (Y 2 O 3 )-graphite composites with a three-dimensional (3D) continuous structure were prepared by using a core-shell design of graphite and ZrO 2 (Y 2 O 3 ). The effect of structure on the friction-reducing and anti-wear mechanisms from room temperature to 700 °C was investigated. During high-temperature friction, abrasive wear and brittle fracture are the main wear mechanisms for ZrO 2 (Y 2 O 3 )-graphite composites with homogeneous composition. For the composites with 3D structure, the continuous ZrO 2 matrix with high load-carrying capacity and the formation of a dense friction layer with self-lubricating and thermal oxidation resistance improve the tribological properties significantly, reducing the coefficient of friction by about 10% and the wear rate by nearly two orders of magnitude when coupled with GH4169 alloys at 600 °C.

CAS / MDL: 7782-42-5
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LANGMUIR · 2023 · IF 3.9

Removal of Formaldehyde and Its Analogues Using a Hybrid Assembly of Pyrene-Modified Hydrazide and rGO: A Negative Carbon Emission and Green Chemical Decomposition Method

Yuru Min,Lei Wang,Chenyao Yuan,Honglei Liu,Xiaole Gong,Mengyu Cao,Jiang-Tao Xu,Jingquan Liu

Indoor gaseous formaldehyde is the main environmental pollutant that can cause fatal threats to human health. A number of physical and chemical methods have been developed to tackle this issue. However, the existing methods are still unsatisfactory to meet the requirement of sustainable development owing to the flaws of low efficiency and reversible or second pollution. Herein, a chemical method based on a nucleophilic reaction between hydrazine and aldehyde that generates the only by-product of H2O is designed for the removal of formaldehyde. 1-Pyrenebutyric hydrazide was synthesized by a simple esterification reaction and then self-assembled on reduced graphene oxide (rGO) with a large surface area by forming π–π stacking to obtain a composite for chemical removal of gaseous formaldehyde under ambient conditions. In a practical test, the formaldehyde removal rate could reach 91% of the theoretical value, which meets the requirement for commercial formaldehyde removal applications. After 10 times recycling, the formaldehyde removal rate still remains as high as 85%. Moreover, the composite could be regenerated in weak acidic media, which greatly reduce the manufacturing cost in practical applications.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

The Structure Evolution of Hydroxyl-Reacted LiBC to Improve the Capacity for Li-Ion Batteries

Hanzhen Peng,Langlang Chen,Yifeng Wang,Bokai Cao,De Li,Yong Chen

As a graphite-like material, the LiBC can deliver a high capacity up to 500 mA h g–1 in Li-ion batteries, which is dependent on the carbon precursor, the high-temperature treatment, and the lithium insufficiency. However, the underlying mechanism is still not clear for the electrochemical reactions of LiBC. In this work, the pristine LiBC was reacted with aqueous solutions of different alkalinity, which was delithiated chemically and retained the layered structure. According to the XPS and NMR results, the B–B bond might be produced through the aqueous reaction or the initial charge process, which can be oxidized (charged) and reduced (discharged) in the electrochemical measurements. In the Li-ion battery, the reversible capacity of LiBC increases evidently with the alkalinity of aqueous solution and significantly rises to a similar value of ca. 285 mA h g–1 under 200 cycles. Therefore, the specific capacity of LiBC should be contributed by the active sites of B–B bonds, which can be significantly increased through the reaction with the hydroxyl ions, and this strategy might be adopted to activate more graphite-like materials.

CAS / MDL: 7782-42-5
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Journal of Physical Chemistry C · 2023 · IF 3.7

Three-Dimensional Network Microstructure Design of the Li4Ti5O12/rGO Nanocomposite as an Anode Material for High-Performance Lithium-Ion Batteries

Ming Wang,Yue He,Wei Hong,Shi Yi Zhang,Chan Xu Yang,Ding Shen,Xiao Liang Wang,Cheng Yan

At present, the wide commercial application of Li4Ti5O12 (LTO) is limited as an anode for lithium-ion batteries because of its poor conductivity and lower rate performance. In this paper, LTO nanoparticles were embedded in a reduced graphene oxide (rGO) conductive network by an in situ electrostatic self-assembly effect using a simple hydrothermal reduction method. The microstructure and electrochemical performance of the LTO/rGO composite were investigated. The highlighted results showed that LTO nanoparticles were combined with rGO nanosheets by a Ti–O–C covalent bond, which was more stable than other bonding methods. At the same time, the addition of rGO not only enriches the structure and increases the specific surface area but also effectively prevents the agglomeration of LTO. The higher conductivity of LTO nanoparticles was bestowed by the rGO three-dimensional (3D) network, causing structural stability and high electrochemical performance. The LTO/rGO composite has high first discharge capacity (643.9 mAh/g at 0.5C), remarkable rate performance (290 mAh/g at 10C), and excellent cycle stability (271.7 mAh/g after the 1000th cycle at 10C) when tested in a half battery. Furthermore, it has higher discharge capacity (181.8 mAh/g at 1C, the first Coulombic efficiency was 90.1%) and excellent cycle stability (142.8 mAh/g after 500 cycles at 20C) when assembled into a full battery as the anode with commercial LiFePO4 (LFP) as the cathode. The lithium storage mechanism of the LTO/graphene composite was further discussed by first-principles calculations. With the addition of graphene to LTO, the electron transport ability was improved and the diffusion energy barrier was reduced. This made the composite expected to become a promising anode material for lithium-ion batteries.

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