ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Jiali Mu,Guifa Long,Xiangen Song,Siquan Feng,Xingju Li,Qiao Yuan,Bin Li,Zheng Jiang,Li Yan,Yunjie Ding
The local coordination environment of central active sites plays a critical role in tuning the catalytic properties of heterogeneous single-metal-site catalysts (HSMSCs). However, carbon supports with inert surface properties provide weak interaction with the active sites, which hamper the effective modulation of the coordination structure of HSMSCs. Herein, this work shows that introducing N and S atoms into carbon support can modify the coordination environment of single-Rh-site and effectively improves the catalytic activity for the methanol carbonylation reaction. The synthesized Rh/AC-NS with single-Rh-site exhibits a high methanol conversion of 88% and a stable acetyl production rate of 2812 h −1 , in contrast with 1285 h −1 of Rh/AC without N- and S- functional groups, and meanwhile remarkably higher than those of Rh/AC-N and Rh/AC-S with only N- or S- functional group under the same mild reaction conditions. As revealed by the experimental result and density functional theory (DFT) calculations, the special combination of N- and S- functional groups offers favorable coordination configuration and also beneficial electronic structure for facilitated CH 3 I oxidative addition and CO insertion steps of single-Rh-site. This work offers new opportunities for rationally tuning the coordination structure of HSMSCs for heterogeneous catalysis.
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2023
·
IF 6.1
Zhongxiu Chen,Ling Li,Zhongshuai Zhao,Ying Zhu,Zhongde Liu
As a highly toxic gas pollutant and also an endogenous gaseous signaling molecule existing in a variety of physiological processes, the rapid and accurate in-field detection of hydrogen sulfide is of great concern. Nevertheless, two drawbacks as for the optical probes for H 2 S detection, taking about a long time to reach the optical signal balance or the low selectivity, always exist. Herein, by using a highly photoluminescent and H 2 S-stimuli responsive silver-based metal-organic frameworks (MOFs): Ag-BDC (BDC = 1, 4-benzene dicarboxylate), we demonstrated that the luminescence intensity of Ag-BDC MOFs was inversely proportional to the concentration of H 2 S due to the Ag–S coordination and the obstruction of ligand-to-metal charge transfer (LMCT) transition process, and there was a quick response time of below 3.0 min. Combined with a simple customized device to separate H 2 S from the sample, the selectivity of the method for H 2 S detection could be greatly improved, and no interference would be caused even if the other sulfur-containing species coexisted. The luminescence probe presented a favorable sensitivity within a linear range of 0.1–1000 μM along with a detection limit of 23.7 nM. When employed to assay the endogenous sulfide level in the human serum and mouse brain tissue, the approach showed recoveries from 96.3% to 102% with relative standard derivation ( RSD ) less than 2.0%. By the integration of the responsive luminescent silver-based MOFs with a simple self-assembled headspace separation device, obviously the present strategy could be beneficial to the development and design of the in-field fast H 2 S measurement, possessing particular advantages in biological systems to eliminate the potential interferences.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Shuaishuai Zhang,Junhua Kuang,Kun Wei,Yuxuan Zhou,Yudian Lei,Nuowen Ma,Huifang Miao,Liuxuan Cao
The wastewater generated by nuclear power plants contains a large number of radioactive substances, including 134 Cs and 137 Cs, which pose significant threats to human health and the environment. It is crucial to remove these radioactive substances from the nuclear waste . A significant challenge we encounter is the effective and selective extraction of cesium ions from wastewater. The wastewater is typically rich in competition ions and spans a wide pH range. In this report, we report a novel manganese silicate/MoS 2 composite material with high adsorption capacity for selectively removing Cs + from aqueous solutions with competition ions. Adsorption behaviors of cesium ions were investigated for composite ratio, adsorbent dosage, contact time, pH and competitive cations. Optimal conditions for the adsorption of cesium ions from aqueous solutions were achieved using a composite ratio of manganese silicate to MoS 2 at 9:1, an adsorbent concentration of 1.0 g L −1 , and a pH of 8 for a duration of 1 h. While the impact of K + and Na + is minimal at lower concentrations, it becomes more pronounced with increasing concentrations. The composite material demonstrates effective performance over the pH range of 2.0–12.0. Experimental data fitted with the pseudo-second-order kinetics and the Langmuir isotherm model suggests a single-layer chemical adsorption process , resulting in a remarkable adsorption capacity of 78.99 mg g −1 . Microscopic analysis reveals the synergistic effect of manganese silicate and MoS 2 . The manganese silicate provides efficient active sites for selective Cs + adsorption, while MoS 2 allows the highly dispersed surface for manganese silicate. This work reveals new insights into the design and synthesis of high-performance Cs + adsorption materials for application in the treatment of nuclear wastewater.
✓ 已验证
产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Jinping Peng,Yihui Huang,Rongwei Fu,Jinqing Lu,Weiquan Wang,Wentao Zhu,Yuxuan Yu,Fan Guo,Haiyan Mai
The target of this study is to gain a deeper understanding of the micro-dissolution process of cellulose in alkaline aqueous solutions and to develop a novel method for extracting cellulose nanofibrils (CNFs). Herein, the dissolution process of cellulose in alkaline aqueous solutions will be controlled by varying the temperature, and the undissolved cellulose will be analyzed to reveal the microscopic dissolution process of cellulose, and a novel process for extracting cellulose nanofibrils (CNFs) will be developed based on the findings. The crystalline structure of cellulose was gradually disrupted as the dissolution progressed, and the crystal form of cellulose changed gradually from cellulose I to cellulose II during the dissolution process, while all undissolved cellulose crystals remained as cellulose I. Cellulose, after its structure is disrupted during the dissolution process, will inevitably decompose into CNFs, and the microscopic dissolution process of cellulose follows a “top-down” dissolution sequence. The CNFs extraction method developed in this study can extract CNFs with high yield (>60 %) in a stable manner, as well as narrow particle size distribution , high crystallinity (>77 %), and good thermal stability . This study enhances the comprehension of the dissolution process of cellulose and paves a possible way for industrialization of CNFs production.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Jun Tang,Jinzhao Huang,Sixuan Zhang,Zehui Liu,Xiaolong Deng
Metal-phase MoS2 (1T-MoS2) is considered a promising candidate as a catalyst for the hydrogen evolution reaction (HER). However, the instability of 1T-MoS2 limits its electrocatalytic activity. Herein, we first synthesized 1T-MoS2 with excellent HER catalytic performance by a simple one-pot hydrothermal strategy of introducing the d-electron-rich transition metal atom Ni into MoS2. A bimetallic monatomic catalyst (Pt@1T-MoS2–Ni) was also prepared by modifying 1T-MoS2–Ni with Pt single atoms (Pt SAs). Experiments show that the electron transfer caused by Ni doping leads to the 1T phase transition, and the modification of Pt SAs further improves the electrical conductivity. These two factors synergistically modulate the electronic composition of MoS2 and increase the number of reactive sites. In consequence, the Pt@1T-MoS2–Ni catalyst exhibits significantly enhanced HER activity, achieving an overpotential as low as 76 mV at 10 mA/cm2 with the corresponding Tafel slope of only 46 mV/dec. Moreover, the current attenuation is negligible within 12 h, surpassing the performance of MoS2. This study offers ideas for improving the efficiency and stability of 1T-MoS2 catalyst designs.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 18
·6554
·
IF 4.6
Yue Chang,Kaili Suo,Yuhang Wang,Xiaona Ren,Jiangli Cao
In this work, a TiO2/In2S3heterojunction film was successfully synthesized using a one-step hydrothermal method and applied in the photocathodic protection (PCP) of 304SS. The octahedral In2S3and In2S3@TiO2nanoparticles combined and coexisted with each other, with In2S3quantum dots growing on the surface of TiO2to form In2S3@TiO2with a wrapping structure. The composite photoelectrode, which includes TiO2with a mixed crystalline phase and In2S3, exhibited significantly enhanced PCP performance for 304SS compared with pure In2S3and TiO2. The In2S3@TiO2/In2S3composites with 0.3 g of P25 titanium dioxide (P25) showed the best protection performance, resulting in a cathodic shift of its OCP coupled with 304SS to −0.664 VAgCl. The electron transfer tracking results demonstrate that In2S3@TiO2/In2S3forms a Z-scheme heterojunction structure. The enhanced PCP performance could be attributed to the synergistic effect of the mixed crystalline phase and the Z-scheme heterojunction system. The mixed crystalline phase of TiO2provides more electrons, and these electrons are gathered at higher energy potentials in the Z-scheme system. Additionally, the built-in electric field further promotes the more effective electrons transfer from photoelectrode to the protected metals, thus, leading to enhanced photoelectrochemical cathodic protection of 304SS.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Li Luo,Shantang Liu,Hanyu Li,Bingquan Xia
Direct methanol fuel cells (DMFCs) have captured increasing attention as promising renewable energy devices. The development of innovative, cost-effective electrocatalysts with superior performance for the methanol oxidation reaction (MOR) holds great significance in promoting DMFCs. In this study, a facile dealloying–electrodeposition method was employed to fabricate stereospecific Ni3S2 nanoflowers on a three-dimensional nanoporous CuAg substrate (Ni3S2@CuAg) for accelerating MOR. The nanoporous CuAg alloy substrate was prepared by dealloying of the metallic glassy (MG) alloy precursor, and the Ni3S2 nanoflowers were in situ grown on the nanoporous CuAg skeleton through a simple electrodeposition process. The novel Ni3S2@CuAg catalysts exhibit outstanding catalytic performance for MOR owing to their preeminent conductivity, large specific surface area, and abundant active reaction sites. Notably, the optimal Ni3S2@CuAg-10 exhibited a superior current density of 340.5 mA cm–2 at 1 V along with good stability (93% current density retention after 2 h) in 1 M KOH and 1 M CH3OH solution. This work presents a novel strategy for designing electrocatalysts with high efficiency and durability for MOR.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 29
·期 1
·234
·
IF 4.6
Fei Tang,Wei Jiang,Jingjing Xie,Deyang Zhao,Yanfeng Meng,Zhenglong Yang,Zhiqiang Lv,Yanbin Xu,Wenjuan Sun,Ziqiao Jiang
Heterostructured materials show great potential to enhance the specific capacity, rate performance and cycling lifespan of lithium-ion batteries owing to their unique interfaces, robust architectures, and synergistic effects. Herein, a polypyrrole (PPy)-coated nanotube-like Mo3S4/CoMo2S4heterostructure is prepared by the hydrothermal and subsequent in situ polymerization methods. The well-designed nanotube-like structure is beneficial to relieve the serious volume changes and facilitate the infiltration of electrolytes during the charge/discharge process. The Mo3S4/CoMo2S4heterostructure could effectively enhance the electrical conductivity and Li+transport kinetics owing to the refined energy band structure and the internal electric field at the heterostructure interface. Moreover, the conductive PPy-coated layer could inhibit the obvious volume expansion like a firm armor and further avoid the pulverization of the active material and aggregation of generated products. Benefiting from the synergistic effects of the well-designed heterostructure and PPy-coated nanotube-like architecture, the prepared Mo3S4/CoMo2S4heterostructure delivers high reversible capacity (1251.3 mAh g−1at 300 mA g−1), superior rate performance (340.3 mAh g−1at 5.0 A g−1) and excellent cycling lifespan (744.1 mAh g−1after 600 cycles at a current density of 2.0 A g−1). Such a design concept provides a promising strategy towards heterostructure materials to enhance their lithium storage performances and boost their practical applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia-Yi Shi,Zhen-Long Wang,Ke-An Wang,Hai-Bin Zhu
The electrochemical reduction of carbon dioxide into energy-carrying compounds or value-added chemicals is of great significance for diminishing the greenhouse effect. However, it is still imperative to replace the less-value anodic oxygen evolution reaction (OER) to improve the technical economy. Herein, we firstly reported a bifunctional CuS/TiO 2 catalyst for both anodic methanol oxidation reaction (MOR) and cathodic carbon dioxide reduction (CO 2 R). The in-built abundant CuS/TiO 2 heterointerfaces are found to boost the CO 2 R and MOR to produce formate. Based on the unique bifunctionality of CuS/TiO 2 , a paired electrosynthesis of formate was performed with a total Faradaic efficiency (FE) of about 170 %, in which the cathodic CO 2 R achieved a formate FE of about 70 %, and the anodic MOR exhibited an almost 100 % formate FE.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Xuening Wang,Zhao Jiang,Jieshu Qian,Wanyi Fu,Bingcai Pan
In the development of nanoenabled technologies for large-scale water treatment, immobilizing nanosized functional materials into the confined space of suitable substrates is one of the most effective strategies. However, the intrinsic effects of nanoconfinement on the decontamination performance of nanomaterials, particularly in terms of structural modulation, are rarely unveiled. Herein, we investigate the structure evolution and decontamination performance of iron (hydr)oxide nanoparticles, a widely used material for water treatment, when confined in track-etched (TE) membranes with channel sizes varying from 200 to 20 nm. Nanoconfinement drives phase transformation from ferrihydrite to goethite, rather than to hematite occurring in bulk systems, and the increase in the nanoconfinement degree from 200 to 20 nm leads to a significant drop in the fraction of the goethite phase within the aged products (from 41% to 0%). The nanoconfinement configuration is believed to greatly slow down the phase transformation kinetics, thereby preserving the specific adsorption of ferrihydrite toward As(V) even after 20-day aging at 343 K. This study unravels the structure evolution of confined iron hydroxide nanoparticles and provides new insights into the temporospatial effects of nanoconfinement on improving the water decontamination performance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Huijie Wang,Jiaye Zhu,Xuhui Ren,Yun Tong,Pengzuo Chen
Tuning coordination environment of single-atom catalysts (SACs) is widely applied for the electrochemical CO 2 reduction reaction (CO 2 RR). However, the influence of the interaction between SACs and support on the catalytic performance are not comprehensive. Herein, taking cobalt phthalocyanine (CoPc) as a conceptual example, a hetero S-atom doping strategy of hollow carbon sphere (S-NHC) is put forward as a carrier, revealing the intrinsic relationship between microenvironment regulation and catalytic activity of single Co-atom. The additional S doping may induce more carbon defect and increases the content of pyrrolic N in the S-NHC sample, leading to stronger electronic interaction of heterogeneous CoPc/S-NHC for boosting CO 2 RR performance. Remarkably, the catalyst achieves a highest CO selectivity of nearly 100% at −0.6 V, and the FE CO are over 90% in a wide potential range from −0.4 to −0.8 V in a flow cell. The maximum power density is high as 2.68 mW cm −2 at 4.7 mA cm −2 for the Zn–CO 2 battery with CoPc/S-NHC cathode. In situ attenuated total reflection infrared (ATR-IR) spectroscopy reveals the formation of key *COOH and *CO intermediates, while the calculation result confirm the optimized Gibbs free energy of these intermediates on CoPc/S-NHC, suggesting the feasibility of the regulation strategy.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Meng Li,Jingxue Sun,Bowen Cong,Shunyu Yao,Gang Chen
The optical and electronic properties of plasmonic semiconductor nanomaterials have attracted a lot of attention. In this study, sulfur vacancies was regulated to achieve carriers density of 10 17 ~ 10 23 cm −3 , with the characteristics of localized surface plasmon resonance (LSPR). Since the excitation of LSPR, the plasma electrons on the semiconductor surface are elevated to a higher energy state. These electrons can overcome the energy barrier between BS and Cd 0.5 Zn 0.5 S (CZS), directly transferred to the conduction band (CB) CZS components as electron donor. This effect may cause more electrons on the semiconductor CB to react with H 2 O to generate more hydrogen. By calculating the Debye length, the scale of the charge effect in the plasma is measured. It can be proved that LSPR is instrumental in the available separation of electrons and holes in semiconductors, and significantly improves the hydrogen production effect of CZS/BS-1.5 nanocomposites. This research furnishes new insights for the construction of efficient and novel polyphase photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）