APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yuqi Zhang,Bang Gu,Zhipeng Zhang,Bohai Wang,Vitaly Ordomsky,Andrei Khodakov,Futing Xia,Wenhao Fang
The catalytic transfer hydrogenation (CTH) of furfural (FF) to furfuryl alcohol (FA) plays a key role in biomass valorization by transforming a renewable platform molecule into a high-value chemical used in resins and polymers. By using alcohols instead of pressurized H 2 , the process enhances safety and energy efficiency. However, the use of non-precious metal single atoms (NPM-SAs) catalysts in CTH of FF to FA under mild conditions remains underexplored. In this study, Co single atoms (Co SAs) were anchored onto a NiO support using a straightforward one-pot NaBH 4 hydrolysis-reduction method, avoiding the high-temperature pyrolysis. The developed Co SAs/NiO catalyst achieved 97% FA selectivity with 99% FF conversion at 120 °C under 1 bar of Ar. FA productivity reached 18.9 mol FA mol Co −1 h −1 and increased to 37.8 mol FA mol Co −1 h −1 when Ar was replaced with an atmospheric H 2 , achieving the highest FA productivity under the milder reaction conditions among all the reported Co-based catalysts. Structural and mechanistic studies using XANES, FT-EXAFS, TEM, in situ DRIFT-IR, and kinetic experiments revealed a strong synergy between Co SAs and the NiO support. Co−O 3 single atoms anchored at oxygen vacancies on the NiO support acted as the key active sites, facilitating the reaction via a “ Meerwein-Ponndorf-Verley ” mechanism. Compared to NiO and Co nanoparticles, Co SAs enhanced FF and isopropanol adsorption with a facilitated FA desorption, lowering the reaction barrier and enhancing the overall efficiency. Additionally, the catalyst demonstrated an excellent stability over eight consecutive cycles without metal leaching and proved effective for CTH of various aldehydes. This study highlights the potential of NPM-SAs catalysts synthesized by a simple method for efficient and selective CTH reactions under mild conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Hui Zhao,Xin-Pu Fu,Wei-Wei Wang,Jin-Cheng Liu,Chun-Jiang Jia
Despite the supported Au demonstrating superior activity in catalyzing various reactions, their stubborn and widespread deactivation issue has long remained unsolved. Therefore, the challenge in current investigations of Au-based catalysts could be divided into two aspects: uncovering the authentic molecular induction for the deactivated evolution and fabricating interfacial structures combining efficiency and stability. In this work, by incorporating NiO x (H) adjacent to small active Au 1 /Au n species, the as-formed 0.5Au-5NiO x (H)/CeO 2 catalyst simultaneously achieved high reactivity ( r = 5.23 mmol CO ·g Au −1 ·s −1 ) toward the water-gas shift (WGS) reaction and remarkable long-term stability with time-on-stream of 100 h at 250 °C, significantly surpassing the reference Au/CeO 2 counterpart as well as the other oxides-supported Au catalysts reported previously. Comprehensive in-situ characterizations and DFT calculations revealed that the CO molecules, rather than H 2 , H 2 O, or CO 2 molecules, are the dominant molecular driver for Au aggregation, correspondingly inducing the degraded catalytic efficiency. Specifically, on the one hand, the strong CO−Au coordination degraded the ejection barrier of Au atoms from Au-Au coordination; on the other hand, the −OH groups as intermediates from H 2 O dissociation, participating in the stabilization of Au species upon the surface, were dynamically consumed by CO molecules. For these regards, the adjacent Ni adatoms promote the sufficient generation of stable −OH groups for stabilizing Au atoms under WGS reaction. As a result, the corresponding Au−Au ejection and Au−O diffusion barriers of as-formed Au n −O(H)−Ni/CeO 2 combinations are significantly enlarged, which thereby boosts the structural stability in the CO-containing atmospheres.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Xinyu Wang,Junhua You,Jiali Ren,Yanjun Xue,Jian Tian,Hangzhou Zhang
In this paper, the Ru/RuS 2 nanoparticles as dual co-catalysts were self-assembled on the surface of g-C 3 N 4 nanotubes (Ru/RuS 2 /g-C 3 N 4 NTs) for photocatalytic H 2 production. The Ru/RuS 2 /g-C 3 N 4 NTs showed greatly enhanced photocatalytic H 2 production activity (1409 μmol·g −1 ·h −1 ), 1.16 times of RuS 2 /g-C 3 N 4 NTs (1212 μmol·h −1 ·g −1 ), 10.51 times of Ru/g-C 3 N 4 NTs (134 μmol·g −1 ·h −1 ), and 82.88 times of the pure g-C 3 N 4 NTs (17 μmol·g −1 ·h −1 ). Besides, the apparent quantum yield value (AQE) of Ru/RuS 2 /g-C 3 N 4 NTs is 3.92% at 370 nm. Ru/RuS 2 as dual co-catalysts are self-assembled on the surface of g-C 3 N 4 NTs and show strong electronic synergistic interaction between the interfaces, reduce Δ G H* of RuS 2 and desorption energy of Ru, and promote the selectivity and activity of HER kinetically and thermodynamically respectively, which exhibits higher photogenerated carrier concentration and lower charge migration resistance than RuS 2 and Ru, showing the synergistic effect to facilitate the generation and migration of carriers and provides active sites for photocatalysis .
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Light-Science & Applications
·
2022
·Vol. 11
·期 1
·1-12
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IF 20.257
Zhang Yan,Miao Shihai,Liang Yanjie,Liang Chao,Chen Dongxun,Shan Xihui,Sun Kangning,Wang Xiao-Jun
The growing demand for spectroscopy applications in the areas of agriculture, retail and healthcare has led to extensive research on infrared light sources. The ability of phosphors to absorb blue light from commercial LED and convert the excitation energy into long-wavelength infrared luminescence is crucial for the design of cost-effective and high-performance phosphor-converted infrared LEDs. However, the lack of ideal blue-pumped short-wave infrared (SWIR) phosphors with an emission peak longer than 900 nm greatly limits the development of SWIR LEDs using light converter technology. Here we have developed a series of SWIR-emitting materials with high luminescence efficiency and excellent thermal stability by co-doping Cr 3+ -Yb 3+ ion pairs into Lu 0.2 Sc 0.8 BO 3 host materials. Benefitting from strong light absorption of Cr 3+ in the blue waveband and very efficient Cr 3+ →Yb 3+ energy transfer, the as-synthesized Lu 0.2 Sc 0.8 BO 3 :Cr 3+ ,Yb 3+ phosphor emits intense SWIR light in the 900–1200 nm from Yb 3+ under excitation with blue light at ~460 nm. The optimized phosphor presents an internal quantum yield of 73.6% and the SWIR luminescence intensity at 100 °C can still keep 88.4% of the starting value at 25 °C. SWIR LED prototype device based on Lu 0.2 Sc 0.8 BO 3 :Cr 3+ ,Yb 3+ phosphor exhibits exceptional luminescence performance, delivering SWIR radiant power of 18.4 mW with 9.3% of blue-to-SWIR power conversion efficiency and 5.0% of electricity-to-SWIR light energy conversion efficiency at 120 mA driving current. Moreover, under the illumination of high-power SWIR LED, covert information identification and night vision lighting have been realized, demonstrating a very bright prospect for practical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Chen Wu,Changyan Zhu,Kangkai Liu,Shaowei Yang,Yu Sun,Kai Zhu,Yueling Cao,Sai Zhang,Sifei Zhuo,Min Zhang,Qiuyu Zhang,Hepeng Zhang
The catalytic hydrogen transfer (CHT) cascade reaction between alcohols and nitro- compounds meets green chemistry yet involves high catalyst requirements. Herein, a hierarchical nano-pyramid structure, in which cobalt single atoms (Co SAs) are deposited on highly dispersed ZnO nanoparticles supported by nitrogen-doped carbon (denoted as Co-ZnO/NC), was designed and obtained through pyrolysis of ZnCo-ZIF. The catalyst exhibited excellent catalytic performance toward the CHT cascade reaction, achieving a high nitrobenzene conversion (94 %), imine selectivity (97 %), and turnover frequency (8.8 h −1 ). This nano-pyramid is a state-of-the-art non-noble-metal catalyst and is comparable to noble-metal catalysts. Experimental and DFT results revealed that the Co SAs supported on ZnO reduced the reaction energy barrier of hydroxyl dehydrogenation, the first and rate-determining step in this heterogeneous catalysis. Furthermore, Co-ZnO/NC exhibits good recyclability and universality. Our findings offer a new catalyst for Schiff base synthesis and aid understanding of the roles of Zn in ZIF-derived carbon catalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Shutong Yang,Weikang Luo,Xianwen Song,Quan Chen,Jingjing Liu,Pingping Gan,Chuntai Liu,Teng Li,Gang Xu,Yi Zhang,Jun Zheng,Yang Wang
The prognosis for traumatic brain injury (TBI) depends largely on prompt hemostasis and effective pharmacologic interventions. Natural all-small-molecule self-gelling powder, integrating the advantages of self-assembled small-molecule hydrogels and powders, is expected to provide timely and effective prehospital management of TBI. However, the synthesis and application of natural all-small-molecule self-gelling powder is still uncharted territory. In this study, an all-small-molecule co-assembled MGF-H 3 BO 3 -RUT (MBR) self-gelling powder is fabricated through the co-assembly of mangiferin (MGF) and rutin (RUT) in H 3 BO 3 /NaOH aqueous solution. Both compounds can bind with boric acid, leading to co-assembling into hydrogels through hydrogen-bonding interactions and π – π stacking. MBR self-gelling powder is then obtained by drying the as-prepared hydrogels, thus integrating hemostasis and pharmacodynamics into one. Remarkably, it displays robust regeneration capabilities, while retaining excellent self-healing properties and injectability after drying-hydration cycles. Moreover, MBR self-gelling powder not only achieves rapid effective hemostasis but also attenuates conspicuously cerebral edema and inflammatory response after TBI by in situ spraying, exhibiting notable neuroprotective effects without discernible toxic side effects. This study provides a novel assembly strategy and application form for self-assembled gel materials originating from natural small molecules, offering promising avenues for the treatment of TBI in the acute phase.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-16
·
IF 17.694
Yang Chuang,Luo Yao,Shen Hao,Ge Min,Tang Jin,Wang Qiaojie,Lin Han,Shi Jianlin,Zhang Xianlong
Strategies to manipulate immune cell co-inhibitory or co-activating signals have revolutionized immunotherapy. However, certain immunologically cold diseases, such as bacterial biofilm infections of medical implants are hard to target due to the complexity of the immune co-stimulatory pathways involved. Here we show that two-dimensional manganese chalcogenophosphates MnPSe 3 (MPS) nanosheets modified with polyvinylpyrrolidone (PVP) are capable of triggering a strong anti-bacterial biofilm humoral immunity in a mouse model of surgical implant infection via modulating antigen presentation and costimulatory molecule expression in the infectious microenvironment (IME). Mechanistically, the PVP-modified MPS (MPS-PVP) damages the structure of the biofilm which results in antigen exposure by generating reactive oxidative species, while changing the balance of immune-inhibitory (IL4I1 and CD206) and co-activator signals (CD40, CD80 and CD69). This leads to amplified APC priming and antigen presentation, resulting in biofilm-specific humoral immune and memory responses. In our work, we demonstrate that pre-surgical neoadjuvant immunotherapy utilizing MPS-PVP successfully mitigates residual and recurrent infections following removal of the infected implants. This study thus offers an alternative to replace antibiotics against hard-to-treat biofilm infections.
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高影响因子
TALANTA
·
2025
·
IF 6.1
Yin-Xia Sun,Xue Bai,Ai-Ping Luo,Yu Sun,Zhe-Peng Deng,Wan-Hong Sun,Wen-Yu Han
Quinolone antibiotics pose a threat to health and the environment due to their difficulty in decomposition and misuse. A novel fluorescence composite material CQD x @Co/Mn-MOF has been developed, which uses cobalt (Co) and manganese (Mn) as metal centers and 1,3,5-triazobenzene as organic ligands. Meaningfully, CQD x @Co/Mn-MOF can be designed as a ratiometric fluorescence sensor for detecting quinolone antibiotics, especially norfloxacin (NFX). In a series of CQD x @Co/Mn-MOF, CQD 6μL @Co/Mn-MOF sensor exhibits good linearity within the NFX concentration range of 1–4 × 10 −5 M, with a detection limit of 0.70 μM. Compared with Co/Mn-MOF, introducing CQDs significantly reduces the detection limit from 3.50 μM to 0.70 μM and increases the detection sensitivity by five times. The CQD 6μL @Co/Mn-MOF sensor exhibits fast response time (2 s), high selectivity and sensitivity to NFX, making it an ideal ratiometric fluorescent sensor for the detection of these antibiotics. Based on its excellent detection performance, the sensor was further applied to the quantitative determination of NFX in chicken, beef and honey samples and satisfactory results were obtained with recoveries ranging from 97.51 % to 108.60 %. In addition, based on CQD 6μL @Co/Mn-MOF test strips, convenient and real-time detection of quinolone antibiotics has been achieved. In conclusion, the CQD 6μL @Co/Mn-MOF ratiometric fluorescent sensor provides a reliable, sensitive and efficient analytical method for the detection and evaluation of trace NFX in food, which is of great significance for ensuring food safety and public health.
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高影响因子
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Deyuan Yang,Ruirui Cui,Chaoyong Deng
Optical thermometry has attracted great attention because it enables accurate temperature measurement in harsh environments due to non-contact temperature measurement. Three-dimensional (3D) lead-free halide perovskites have a great application potential in this field, due to its outstanding luminous properties and stability. In this work, the Sb 3+ and Er 3+ are introduced in Cs 2 NaYCl 6 double perovskites (DPs). The Sb 3+ doping Cs 2 NaYCl 6 DPs exhibits bright blue emission from the Sb 3+ activated self-trapped excitons (STEs) and Sb 3+ ,Er 3+ co-doped Cs 2 NaYCl 6 has efficient green emission with excellent photoluminescence quantum yields (PLQY) of 81.1% because of the presence of energy transfer from self-trapped excitons to Er 3+ ions. Excitingly, the ratio between the fluorescence intensity at 524 nm and 550 nm (FIR( I 524 nm / I 550 nm )) and the ratio between the fluorescence intensity at 524 and 456 nm (FIR( I 524 nm / I 456 nm )) both have a high correlation with temperature in the range of 298–473 K. The maximum of relative sensitivity values reach to 1.18%/K ( I 524 nm / I 550 nm ) and 1.19%/K ( I 524 nm / I 456 nm ) at 298 K, respectively. The outstanding temperature sensitivity suggests that the Sb 3+ ,Er 3+ co-doped Cs 2 NaYCl 6 has enormous application potential in ratiometric optical thermometry.
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Results in Chemistry
·
2025
·
IF 4.2
Fuhua Wei,Peng Chen,Qinhui Ren,Qin Zhang,Wei Shang,Diaodiao Zhang,Min Li,Zhao Liang
The Co/Zn-MOFs material was synthesized successfully via the solvothermal method and then underwent calcination at 900 °C. To investigate its structural properties, multiple characterization techniques were applied, such as scanning electron microscopy (SEM), Fourier-transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), and nitrogen adsorption-desorption isotherms. These analyses aimed to assess the features of the carbon material for its efficacy in minocycline removal. The experimental findings demonstrated that the ideal conditions for maximizing minocycline adsorption on the carbon material obtained from Co/Zn-MOFs comprised a dosage of 20 mg, a solution concentration of 50 ppm, and a pH level of 10. Furthermore, kinetic studies revealed that the pseudo-second-order model accurately represented the experimental data. In conclusion, this research underscores the remarkable adsorption capability of the carbon material derived from Co/Zn-MOFs for minocycline, indicating potential applications in environmental cleanup and presenting an innovative approach for environmental preservation.
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COMPARATIVE BIOCHEMISTRY AND PHYSIOLOGY C-TOXICOLOGY & PHARMACOLOGY
·
2025
·
IF 4.3
Yuxuan Luo,Zheng Zhang,Xuewei Li,Zile Zhuang,Yihan Li,Xinya Wang,Changqing Liao,Lujia Chen,Qizhi Luo,Xuncai Chen
Microplastics (MPs) are ubiquitous environmental pollutants that have garnered significant attention due to their small particle size, resistance to degradation and large specific surface area, which makes it easy to adsorb various pollutants, particularly heavy metals. Arsenic (As), a common metal poisons, poses significant risks due to its widespread industrial use. When MPs and As co-exist in the environment, they can exert combined toxic effects on organisms, affecting various systems, including the nervous system. However, research on the reproductive damage caused by the co-exposure to MPs and As is limited, and the toxic effects and mechanisms remain unclear. In this study, we investigated the co -exposure of polystyrene microplastics (PSMP) and As on female zebrafish to evaluate the reproductive toxicity and transgenerational effects. The results revealed that the combined exposure exhibited elevated reproductive toxicity, resulting in reduced gonadal indices, abnormal oocyte maturation, and disrupted sex hormone levels, as evidenced by an increased E2/T ratio. Metabolomics analyses revealed that the co-exposure to PSMP and As primarily affected pathways involved in aminoacyl-tRNA biosynthesis, sphingolipid metabolism, linoleic acid metabolism, galactose metabolism, and amino sugar and nucleotide sugar metabolism. These pathways are associated with oxidative stress, lipid synthesis, and sex hormone synthesis. Importantly, the combined exposure group exhibited more pronounced effects on offspring development compared to the alone treatment group, characterized by increased mortality rate, decreased hatching rate, and reduced heart rate. These findings provide evidence that co-exposure to MPs and As damages the reproductive system and adversely affects offspring growth and development.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yongdie Zhao,Xiaohao Liu,Rui Diao,Dongxu Yan,Fenglei Qi,Peiyong Ma
Selective hydrogenation of fatty acids is an important method for the preparation of long-chain alkanes and fatty alcohols. Herein, a series of bimetallic catalysts with different Fe/Co ratios were prepared by using phosphoric acid-activated biochar as a support. The anchoring effect of P-containing functional groups in the support greatly improves the sintering resistance of the metals. The conversion pathway of stearic acid (SA) can be regulated by controlling Fe doping and the reduction temperature. The reduction of Fe1Co3/PAC at 400 °C can selectively regulate the hydrodeoxygenation pathway of SA. At 250 °C and 4 MPa, SA was almost completely converted to long-chain alkanes. Mechanism study shows that Fe doping increases the hydrogenation site CoO and dehydration site Fe–O–P in catalysts. However, by further increasing the reduction temperature, the metal phosphides formed in the catalyst can significantly enhance the dehydrogenation of octadecanol and decarbonylation of octadecaldehyde.
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