Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 29
·15543-15553
·
IF 14.511
Weibin Chen,Yuxin Xie,Xuehui Gao,Lei Li,Zhan Lin
Multiple electronic structure modification is propitious for constructing strong metal–support interaction and then improving the electrocatalytic activity of supported catalysts, yet remains a great challenge due to the lack of facile protocols. Herein, we report a CoIr alloy supported on two dimensional (2D) graphitic-N doped carbon (CoIr@CN) through a one-step annealing process from an Ir-doped 2D Co-MOF, which exhibits a remarkably reduced Ir loading (2.69 wt%) and enhanced electrocatalytic activity for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Ir plays an essential role of optimizing the properties of metal nanoparticles and simultaneously effecting the calcining process to adjust the N-doping structure, eventually modulating the synergetic effect between alloy nanoparticles and the N-doped carbon support. Owing to the positive effect of such multiple electronic structure optimization, the electron transfer between alloy nanoparticles and N-doped carbon is promoted to enable more moderate adsorption energies of reaction intermediates in both the OER and HER. Impressively, CoIr@CN exhibits a low OER/HER overpotential of 269 mV/70 mV to achieve a current density of 10 mA cm−2 in 1.0 M KOH, and 25 mV in 0.5 M H2SO4 for HER, as well as a negligible decay of catalytic activity after long-term stability measurements for OER/HER. This study offers an effective way for designing strong metal–support interaction through multiple electronic structure modification, which effectively improves the OER/HER performance of supported catalysts.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2020
·
IF 3.306
Xiaoye Wen,Li Yan,Zhefeng Fan
A novel and simple probe (denoted LN-1) with AIE property based on malononitrile and 4-diethylaminobenzaldehyde was designed and synthesized. The use of two different mechanisms for the independent detection of Fe 3+ and CN − is more convenient and efficient than the continuous detection of anions and cations. The detection mechanism was verified by mass spectrometry (MS), nuclear magnetic resonance (NMR) spectrum, and particle size distribution. Under optimized experimental conditions, excellent calibration curves were obtained for the LN-1-Fe 3+ and the LN-1-CN − with detection limits of 0.17 and 0.39 μM, respectively. This method was successfully applied to detect the content of Fe 3+ and total inorganic iron in actual samples. Owing to its low cytotoxicity, good biocompatibility, and enhanced orange emission in aqueous solution, the LN-1 was successfully applied for CN − imaging in live cells. In addition, Fe 3+ and EDTA incorporation into the LN-1 changed the fluorescent intensity, which is beneficial in constructing ultrasensitive INHIBIT logic gate.
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EcoMat
·
2024
·
IF 10.7
Junming Shi,Guoyang Gao,Can Jin,Hongqing Wu,Weizhen Wang,Yulong An,Zhen Zhou,Zhanhua Huang,Wenshuai Chen
Value-added conversion of lignocellulose is a sustainable approach. Photo-refining biomass is in line with current environmental protection strategies. However, photo-reforming biomass suffers from poor catalyst stability and low conversion efficiency. Here, we designed fructose as a lignocellulosic model. The heterogeneous structure of Prussian blue coating was constructed with a special covalent bond structure of Co CN Zn. This structure has a catalytic conversion mechanism that can accelerate electron transfer. Fructose was simultaneously converted to value-added platform compounds (5-HMF and formic acid) and gaseous fuels (CO, CH 4 ) with a conversion rate of up to 92.5%, which is more than 1.7 times than that of catalysts without adding Prussian blue. Hydrogen transfer and carbon transfer on the carbon atoms of fructose facilitates the production and accelerates the spillover of CO from formic acid. This work provides new ideas for the development of Prussian blue catalysts and the conversion of pentose.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
·
IF 7.7
Xiaotong Wang,Tongtong Ye,Shaohui Geng,Shuna Ren,Xuming Zhao,Lihua Chen
A dual-signal strategy was developed based on a coordination reaction between iron(II) ions (Fe 2+ ) and potassium hexacyanoferrate(III) (K 3 [Fe(CN) 6 ]) to distinguish between brucella vaccine and wild strain. Utilizing metal-organic frameworks (MOFs), MOF Al (aluminum) @Fe 2+ @P 1 and MOF Fe @P 2 were synthesized and affixed to a hyaluronic acid (HA)-doped electrode. Hairpin probe 1 (P 1 ) has a common sequence (P 1 ') recognizing a fragment (T 1 ) in vaccines and wild strains. In contrast, hairpin probe 2 (P 2 ) has a differential sequence (P 2 ') only targeting a specific fragment (T 2 ) in the wild strain. Experimental findings indicated that activation of T 1 led to the dissociation of P 1 from MOF Al @Fe 2+ @P 1 , which released Fe 2+ into a buffer containing trace Fe 2+ . Following this, the addition of hydrogen peroxide (H 2 O 2 ) and K 3 [Fe(CN) 6 ] resulted in the formation of KFe[Fe(CN) 6 ] (PB). In contrast, specific activation of T 2 caused the detachment of P 2 from MOF Fe , thereby exposing its catalytic site. In H 2 O 2 , this catalytic site facilitated the conversion of trace Fe 2+ in buffer to Fe 3+ , with no PB generated after the addition of K 3 [Fe(CN) 6 ]. Simultaneous activation of T 1 and T 2 promoted the oxidation of Fe 2+ released from MOF Al by the exposed catalytic site of MOF Fe . The ratio of K 3 [Fe(CN) 6 ] to PB exhibited dynamic changes. Specifically, the ratio below 2.37 ± 0.05 indicated a Brucella-positive sample, whereas a ratio under 0.9 ± 0.02 suggested a sample derived from the vaccine. The scarcity of dual-signal sensors employing coordination reactions underscores the significance of this approach. Moreover, it addressed the challenges associated with brucella detection, demonstrating robust analytical performance.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 24
·7274-7284
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IF 7
Yulin Kong,Yawei Xiao,Shutao Zhang,Liang Chen,Zhaoping Liu,Yude Wang
Aqueous zinc-ion batteries (AZIBs) are considered promising energy storage devices for future large-scale energy storage systems due to their high safety, low production cost, and non-combustibility. However, low operating voltage and energy output are still drawbacks in their practical applications. Herein, we develop a cubic aluminum hexacyanoferrate/graphene high-voltage cathode material for rechargeable AZIBs, and it exhibits an activation process and can deliver a high output voltage of 1.8 V (vs. Zn/Zn2+) with a specific energy density of 125.56 W h kg−1. The voltage is increased by stretching the Fe–C bonds in the Fe–CN–Al covalent structure. The reversible phase transformation between cubic AlFe(CN)6 and cubic–orthorhombic–monoclinic Zn0.5AlFe(CN)6 occurs with the intercalation/extraction of zinc ions, and the coordination environment of Al plays a decisive role in this key process. This work will provide a feasible reference for the structural design of high-voltage Prussian blue analog cathode materials.
研究领域:
材料科学
·
电化学
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Pengfei Zhu,Xiaolong Wu,Xingyang Xiao,Ming Duan,Dan Luo,Jinru Lin
In this work, Bi 12 O 17 Cl 2 and ZIF-8 were synthesized via a facile in-situ precipitation method, while ZnO-CN was obtained through the pyrolysis of ZIF-8. Then, a novel Bi 12 O 17 Cl 2 /ZnO-CN composite catalyst with Z-scheme heterojunction was prepared by mechanical mixing-low temperature activation method. When the ZnO-CN is pyrolyzed at 550 ℃ and accounts for 10 wt% in the Bi 12 O 17 Cl 2 /ZnO-CN composite, the composite exhibited a significantly higher degradation rate for levofloxacin hydrochloride (LVX) (94.50%) compared to Bi 12 O 17 Cl 2 (67.30%) and ZnO-CN (36.80%), while also achieving a high removal rate of Cr(VI) under acidic conditions (92.00%). And the toxicity of LVX to wheat decreased significantly after photocatalytic degradation. Meanwhile, the Bi 12 O 17 Cl 2 /ZnO-CN has good universality, salt resistance and reuse stability. The experimental results of sample characterization show that the improved photocatalytic performance of Bi 12 O 17 Cl 2 /ZnO-CN composite can be attributed to the high-efficiency separation of electron-hole pairs (e - -h + ), enhanced light absorption in the visible region, increased specific surface area and active sites. Both the free radical capture experiment and electron paramagnetic resonance (EPR) test indicate that •O 2 - and h + are the primary active species in the process of degrading LVX by Bi 12 O 17 Cl 2 /ZnO-CN. Combined with mechanism exploration experiment and iquid chromatography-mass spectrometry (LC-MS) analysis, a possible direct Z-scheme heterojunction electron transfer mechanism and photocatalytic degradation pathways for LVX was proposed. This work enhances the photocatalytic performance of Bi 12 O 17 Cl 2 and provides an idea for antibiotic or Cr(VI) wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Min Wang,Dehua Xin,Wei Zhang,Dan Luo,Guoqiang Tan
The optimization of the photogenerated carriers’ relaxation dynamics process is critical for the improvement of photocatalytic performance. Herein, a ternary heterojunction with multilevel charge transfer channels was constructed by coupling plasma Ag, nitrogen vacancies carbon nitride (NVs-CN) and Bi 2 O 2-δ CO 3 . Ag/NVs-CN/Bi 2 O 2-δ CO 3 heterojunction showed the S-scheme mechanism, which not only promoted the interfacial charge transfer, but also enhanced the driving force for redox reactions. The defect states induced by nitrogen vacancies and oxygen vacancies provided an additional energy level platforms for hot electrons relaxation of plasma Ag, resulting in the improved separation efficiency and utilization rate of the high-energy hot carriers. Hence, the prepared Ag/NVs-CN/Bi 2-δ O 2 CO 3 heterojunction exhibited the markedly boosted full-spectrum driven catalytic activity for antibiotics degradation. 80.5% and 83.8% of tetracycline and ciprofloxacin could be mineralized into H 2 O and CO 2 by the optimal heterojunction under visible light irradiation, and the corresponding mineralization efficiencies could reach 81.7% and 81.5% under NIR light irradiation. The proposed multichannel charge transfer mechanism provided a new insight into the design and preparation of high-active full-spectrum responsive heterojunction photocatalysts.
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CHINESE CHEMICAL LETTERS
·
2014
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IF 1.178
Dong-Shun Deng,Guo-Qiang Han,Xiao Zhu,Xuan Xu,Yu-Tong Gong,Yong Wang
Mesoporous N-doped carbon supported palladium catalyst Pd@CN 0.132 was able to efficiently catalyze unprotected indole to indoline under mild conditions. In the aqueous system, a selectivity of 100% and conversion of 96% was achieved under 313 K and atmospheric hydrogen gas.
研究领域:
催化
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有机化学
·
材料科学
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Small Methods
·
2022
·Vol. 6
·期 8
·2200404
·
IF 15.367
Chun-Mei Xu,Jian Peng,Xiao-Hao Liu,Wei-Hong Lai,Xiang-Xi He,Zhuo Yang,Jia-Zhao Wang,Yun Qiao,Li Li,Shu-Lei Chou
Prussian blue analogues (PBAs) have attracted extensive attention as cathode materials in sodium-ion batteries (SIBs) due to their low cost, high theoretical capacity, and facile synthesis process. However, it is of great challenge to control the crystal vacancies and interstitial water formed during the aqueous co-precipitation method, which are also the key factors in determining the electrochemical performance. Herein, an antioxidant and chelating agent co-assisted non-aqueous ball-milling method to generate highly-crystallized Na 2- x Fe[Fe(CN) 6 ] y with hollow structure is proposed by suppressing the speed and space of crystal growth. The as-prepared Na 2- x Fe[Fe(CN) 6 ] y hollow nanospheres show low vacancies and interstitial water content, leading to a high sodium content. As a result, the Na-rich Na 1.51 Fe[Fe(CN) 6 ] 0.87 ·1.83H 2 O hollow nanospheres exhibit a high initial Coulombic efficiency, excellent cycling stability, and rate performance via a highly reversible two-phase transition reaction confirmed by in situ X-ray diffraction. It delivers a specific capacity of 124.2 mAh g −1 at 17 mA g −1 , presenting ultra-high rate capability (84.1 mAh g −1 at 3400 mA g −1 ) and cycling stability (65.3% capacity retention after 1000 cycles at 170 mA g −1 ). Furthermore, the as-reported non-aqueous ball-milling method could be regarded as a promising method for the scalable production of PBAs as cathode materials for high-performance SIBs.
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PubMed
高影响因子
Food Bioscience
·
2026
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IF 6.2
Zixian Xia,Xiaoyan Guan,Rui Liu,Yeting Wu,Yingying Li,Mengmeng Liu,Yifeng Ding,Xiaohong Wang,Youyou Lu
Bifidobacterium faces major challenges in the gastrointestinal tract, including inactivation under acidic conditions and insufficient targeted release. In this study, three novel heterologous dual-protein complex systems were constructed by lactoferrin (LF) with α-lactalbumin (ALA), β-lactoglobulin (BLG), casein (CN). Subsequently, sodium alginate (SA) -cross-linked gel microcapsules loaded with these dual-protein complexes and B. animalis F1-7. The optimal preparation conditions for the dual-protein were as follows: ALA/LF = 1.5, 50 °C; BLG/LF = 2, 50 °C; CN/LF = 0.5, 25 °C. Incorporation of SA and endogenous emulsification method enabled efficient encapsulation of B . animalis F1-7, achieving encapsulation efficiency exceeding 90%. B. animalis F1-7@SA-(LF-ALA/BLG/CN) exhibited strong acid resistance, favorable intestinal responsiveness, and significantly improved microbial viability. The microcapsules enhanced gastric acid tolerance primarily through a spatial barrier effect, while the incorporation of dual-protein components contributed to matrix structural reinforcement and digestion-responsive release behavior. This integrated “physical protection-structural modulation” strategy also conferred excellent 28-day storage stability. In vitro experiments by mice/human feces, combined with 16S rRNA and metabolomics analysis, revealed that the composite microcapsules effectively regulated the structure of the microbial community and altered metabolite profiles (e.g. , pathways involved in nitrogen metabolism). Overall, this study provided reproducible preparation parameters and a theoretical basis for SA-based dual-protein composite encapsulation delivery systems, and offered a promising strategy to address the coordinated challenges of activity, controlled release, and storage stability of sensitive food bioactive microorganisms or nutrients.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 11
·1-12
·
IF 2.4
Lu Wei,Zhou Liang
Photocatalytic regeneration of nicotinamide adenine dinucleotide (NADH) is indispensable for the sustainability of enzyme-driven industrial processes. In this study, we developed a Z-scheme heterogeneous photocatalyst consisting of CdS and g-C 3 N 4 , which markedly enhanced visible-light absorption and photogenerated charge separation efficiency, and applied it to an in situ visible-light-driven NADH regeneration system. The synthesized catalyst afforded an exceptional NADH regeneration yield of 97.88% within just 15 min. Additionally, enzyme activity assays utilizing alcohol dehydrogenase (ADH) demonstrated that 67.60% of NAD + was successfully converted into the enzymatically fraction, 1,4-NADH. Furthermore, formate dehydrogenase (FDH) immobilized on ZIF-8 was integrated into this NADH regeneration system, enabling highly sustainable biosynthesis of formic acid. During a 2 h continuous reaction, the integrated system successfully accumulated a total formic acid concentration of 0.88 mM. This novel Z-scheme photocatalytic system thus presented a highly effective solution for regenerating active NADH, providing valuable insights and promoting the development of photocatalysis-driven enzymatic systems for sustainable solar-to-chemical energy conversion. Graphical
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Yunchao Feng,Sishi Long,Guihua Yan,Wenlong Jia,Yong Sun,Xing Tang,Zehui Zhang,Xianhai Zeng,Lu Lin
Developing the active and environmentally friendly non-noble nano-catalysts is highly desired to transform biomass-derived platform into value chemicals. Herein, we report a low-cost and sustainable cobalt/nitrogen-doped carbon catalyst containing both metallic Co and Co-N components exhibits satisfying activity for the oxidative esterification of 5-hydroxymethylfurfural and other investigated alcohols in methanol without the base additive under mild conditions. Experimental results show that an appropriate ratio of Co to Co-N is responsible for the high activity of the Co/Co-N/CN catalysts towards oxidative esterification. Theoretical computational results demonstrate that the Co/Co-N group synergistically promotes electron transfer from the Co adatom to the surface oxygen atoms, facilitates O 2 adsorption and activation on the Co sites, and further reduces the energy barrier for the oxidation of alcohols to aldehydes, all of which contribute to the overall activity of oxidative esterification of alcohols to the corresponding esters. In addition to exhibiting superior intrinsic activity, the as-prepared Co/Co-N/CN catalyst also shows excellent stability and recyclability.
研究领域:
催化
·
材料科学
·
化学工程
·
环境科学
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高影响因子
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