ACS Applied Materials & Interfaces
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2021
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IF 9.229
Lin Ma,Jian Gao,Chen Huang,Xiao Xu,Lu Xu,Renhao Ding,Hongliang Bao,Ziqiang Wang,Gang Xu,Qingnuan Li,Pengyang Deng,Hongjuan Ma
Metal–organic frameworks (MOFs) with a high surface area and excellent stability are potential candidates for uranium (U) adsorption. Amidoxime (AO) is the most widely used functional group to extract U, which is usually introduced into MOFs by two-step post-synthetic methods (PSMs). Herein, MOF UiO-66-NH-(AO) was obtained by a one-step PSM with amidoximation from UiO-66-NH-(CN), which was synthesized by a new organic ligand of 2-cyano-terephthalic acid and whose morphology was octahedron and could be well controlled with the new ligand. The one-step PSM can greatly maintain the octahedron of the MOFs. What is more, UiO-66-NH-(AO) showed good adsorption performance for U, the adsorption equilibrium was obtained within 1500 min, and the adsorption capacity of U was calculated to be 134.1 mg/g according to the Langmuir model. It also had excellent selectivity for U in the presence of high concentrations of vanadium (V), ferrum (Fe), magnesium (Mg), calcium (Ca), and zirconium (Zr). The adsorption capacity of U in natural seawater was determined to be 5.2 mg/g within 8 days. The recyclability of UiO-66-NH-(AO) in simulated seawater was demonstrated for at least four adsorption/desorption cycles. The binding mechanism was investigated by the extended X-ray absorption fine structure spectroscopy, revealing that U binding occurs in a fashion η2 motif. This study provides a reliable idea for the modification of MOFs and the potential for MOF-based materials to extract U from seawater.
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Journal of Physical Chemistry C
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2017
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IF 4.536
Wanfeng Li,Fang Zhang,Xingde Xiang,Xiucheng Zhang
Nickel-based ferrocyanides have attracted wide interest as cathode for aqueous sodium-ion batteries in fields of sustainable energies such as wind and solar, owing to excellent cycling stability and high-rate capability. However, they suffer from low specific capacities (∼60 mAh g–1). Herein, Na2Ni0.4Co0.6[Fe(CN)6] nanocrystallites are reported for the first time as high-capacity cathode for aqueous sodium-ion batteries. Its electrochemical properties and redox mechanism have been understood by combining the X-ray diffraction technique, Fourier-transform infrared spectroscopy, cyclic voltammetry, electrochemical impedance microscopy, and charge/discharge measurements. It is revealed that the material undergoes a reversible three-step single-phase reaction mechanism during Na extraction through sequential electrochemical oxidation of nitrogen-coordinated Co2+ ions and carbon-coordinated Fe2+ ions and achieves superior electrochemical performance with a high reversible capacity of 85 mAh g–1 at 0.5 C, an average operating potential of 0.62 V (vs Ag/AgCl), and a high capacity retention of 90% after 100 cycles. The combination of high specific energy and good cycling performance enables the Na2Ni0.4Co0.6[Fe(CN)6] material exhibiting promising application for high-performance aqueous sodium-ion batteries.
研究领域:
电化学
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储能
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材料科学
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电池技术
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Journal of Energy Storage
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2026
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IF 10.7
Kaixin Xie,Xiaobo Chen
In the pursuit of advanced energy storage solutions, materials featuring high porosity, robust redox activity, and abundant electrochemically accessible sites are highly attractive candidates for next-generation supercapacitor electrodes. In this study, a binder-free positive electrode material consisting of porous MnCo 2 O 4 particles directly coated onto carbon cloth (MnCo 2 O 4 @CC) was synthesized via a straightforward hydrothermal process followed by thermal treatment. Additionally, the incorporation of redox additives into electrolytes has been identified as a promising approach to elevate electrochemical supercapacitor performance. To this end, we designed an aqueous asymmetric supercapacitor (ASC) system utilizing MnCo 2 O 4 @CC and activated carbon (AC) electrodes, where potassium ferricyanide (K 3 [Fe(CN) 6 ], denoted as KFCN) was introduced as an electrolyte additive to augment pseudocapacitive behavior. The electron migration mechanisms and charge storage dynamics of MnCo 2 O 4 @CC in a KOH + KFCN electrolyte were systematically investigated. The MnCo 2 O 4 @CC electrode immersed in a 3 M KOH + 0.05 M KFCN solution exhibited a high specific capacitance of 2206.7 F g −1 at 1 A g −1 , along with low resistance characteristics and exceptional cycling durability. A complete aqueous MnCo 2 O 4 @CC//KOH + KFCN//AC ASC was assembled, demonstrating enhanced specific capacitance, extended cycle life (94.5% capacitance retention after 10,000 cycles), and an ultrahigh energy density of 79.9 Wh kg −1 at 799.6 W kg −1 . These findings provide significant electrochemical insights and demonstrate the great potential of the MnCo 2 O 4 @CC-KOH + KFCN system for next-generation supercapacitor applications.
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GREEN CHEMISTRY
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2026
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IF 10.6
Zhe Zheng,Yushun Han,Weikang Ling,Min Hong,Jiliang Ma,Runcang Sun
Noble metal catalysts face multiple challenges in photocatalytic applications, including high cost, limited active sites, and insufficient stability. In contrast, high-entropy alloys (HEAs) present a promising alternative due to their distinctive high-entropy effect, lattice distortion, sluggish diffusion, and cocktail effect. In this study, a MoMnZrTmBa HEA cocatalyst was rationally designed and integrated in situ with carbon nitride (CN) to construct a Schottky heterojunction. Within this architecture, the CN substrate acts not only as a stabilizing scaffold that promotes the dispersion and exposure of HEA active sites, but also as an electron donor to modulate the electronic structure. The interfacial Schottky barrier enables directed separation and migration of photogenerated charge carriers. Meanwhile, the synergistic interactions among the multiple HEA components provide abundant active sites, substantially enhancing the photocatalytic efficiency. Notably, the optimized H/C-15 catalyst delivered outstanding performance in the selective oxidation of xylose, achieving a high xylonic acid yield of 67.86% and a CO production rate of 2534.52 μmol g−1 h−1. Outdoor experiments under concentrated sunlight and 30 consecutive recycling tests further demonstrated excellent structural stability and practical viability of the system. This work underscores the potential of HEAs in photocatalytic biomass valorization and provides a strategic framework for their rational design.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Xuejian Zhang,Yongjie Wang,Shuanghong Zhao,Shuai Zhang,Xinhua Gao,Kangzhou Wang,Subing Fan,Qingxiang Ma,Tian-Sheng Zhao,Jianli Zhang
Although Fe-based Fischer-Tropsch synthesis catalysts exhibit advantages in linear α-olefins (LAOs) synthesis, how to promote C C coupling and inhibit the secondary hydrogenation of olefins remains a challenge. Herein, we report an N-doped carbon supported Fe-based catalyst fabricated via a self-templated combustion activation strategy and impregnation method, which enables the highly selective conversion of syngas to LAOs. Systematic characterizations revealed that sodium citrate-assisted activation optimized the pore structure of the supports, facilitated the transformation of N configurations and enhanced the relative content of pyrrolic N. Pyrrolic N regulated the surface electron density of the active sites, which enhanced the adsorption and activation of CO and facilitated the C C coupling reactions, leading to an increase in C 5 + selectivity from 25.64% to 40.71%. Meanwhile, the electronic effect of pyrrolic N effectively weakened the interaction between olefins and active sites, thereby suppressing the secondary hydrogenation of olefins. The Fe/CN(Act.)-550 catalyst exhibited LAOs selectivity increasing from 29.89% over Fe/CN550 catalyst to 70.15%. The catalyst outperforms most previously reported results and maintains stability during 120 h long-term operation without significant sintering or coking. This work provides new insights for the design of catalysts for the highly efficient conversion of syngas to LAOs.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Xiang Liu,Haoyu Chen,Xiaojun Hu,Jing Liu,Xiaohua Zhu,Youyu Zhang,Meiling Liu
Excessive presence of cyanide in various environmental and biofluids poses a significant threat due to its highly toxic nature and potential threat to living organisms. Nevertheless, a multitude of current techniques encounter difficulties in sensitivity and selectivity issues. Inspired by the Cu-N active sites in natural laccase, we propose novel copper-based porphyrin metal-organic frameworks (Cu-TCPP) nanosheets that act as potent laccase mimics, which has been firstly used for the ultra-sensitive cyanide detection. The electron-rich nature, strong reductivity, and Cu-ion coordination ability of cyanide ions (CN - ) specifically enhances the mimic activity of Cu-TCPP. The incorporation of CN - also increases the Cu + /Cu 2+ ratio and oxygen vacancies, accelerates the interaction between Cu-TCPP and its substrates, enhancing the electron transfer and improving oxygen activation efficiency and catalytic cycling. Notably, the regulatory effect of CN - is concentration-dependent, enabling sensitive CN - detection. To address potential interferences from the inherent color and UV absorption of the nanomaterials, a post-reaction centrifugation technique has been introduced, allowing for accurate measurement with improved resolution and sensitivity. The innovative strategy of utilizing a cofactor to regulate the laccase mimics activity provides fresh insights into the design of advanced nanozymes and offers an alternative method for detecting cofactors, facilitating broader applications in various fields.
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TOPICS IN CATALYSIS
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2026
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IF 3.7
Wu Jundao,Huang Zeai,Zhang Fan,Liu Jiayi,He Yi,Hu Wei,Tang Xiao,Zairov Rustem,Sinyashin Oleg G.
The substantial presence of nitrogen oxides (NO and NO 2 ) in outdoor environments detrimentally impacts natural ecosystems and exerts significant influence on urban climates. Conventional NO x treatment methods frequently suffer from challenges such as harsh reaction conditions and high energy consumption. Consequently, the development of advanced photocatalytic systems to efficiently degrade NO x while minimizing the formation of toxic byproducts represents a critical challenge in environmental catalysis. In this study, a novel ternary composite material (5% Mo-CN/InP-NBOC) was constructed via hydrothermal synthesis and surface modification strategies, achieving 42% NO oxidation efficiency under visible light irradiation with a mere 0.9% NO 2 generation rate. This performance demonstrates efficient photocatalytic NO oxidation while effectively suppressing NO 2 production. Systematic characterization techniques, including XRD, TEM, and XPS, confirmed the successful integration of InP quantum dots (5–10 nm) and amorphous Mo-CN onto NBOC nanosheets, forming an intimate heterojunction structure. PL and ESR analyses revealed that Mo-CN enhances charge carrier separation and governs the NO oxidation process through the activation of dual free radical pathways (⋅O 2 − and ⋅OH). This work establishes a “quantum dot-primary catalyst-cocatalyst” ternary collaborative design paradigm, providing experimental evidence and theoretical models to address the challenges of synergistic optimization among activity, selectivity, and stability in photocatalytic NO x treatment.
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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
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2022
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IF 5.168
Han Jia,Daofan Wang,Qiuxia Wang,Jiajun Dai,Qiang Wang,Shijie Wen,Zhe Wang,Bowen Wang,Xincan Jiang,Xu Li,Kaihe Lv
Mixed nanoparticle stabilized Pickering emulsion is a novel research topic, which has been attracted more attention. In the present study, the novel amphiphilic GO-Janus SiO 2 -Cn nanoparticles (GOJS-Cn, n represents the number of carbon atoms in the modified alkyl chain) were successfully fabricated for the first time and investigated their ability in stabilizing Pickering emulsions for enhancing oil recovery. Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) were employed to determine the successful fabrication of the GOJS-Cn. The optical microscopy was utilized to directly observe the GOJS-Cn (n = 0, 3, 8, and 12) stabilized emulsions and the static multiple light scattering was employed to further evaluate its stability quantitatively. It was found that the GOJS-C12 displayed the greatest ability to stabilize emulsions, even in high salinity (10 4 mg/L NaCl/MgCl 2 /CaCl 2 /AlCl 3 ) and temperature (90 °C). Then, the interfacial tension, water contact angle, and dilatational measurements were conducted to reveal the mechanism of the GOJS-C12 superior emulsifying ability. The amphiphilic GOJS-C12 with great amphiphilicity spontaneously adsorbed at oil-water interface to promote the formation of rigid interfacial film, which was essential for the long-term stability of emulsion . Moreover, the core flooding tests reflected the GOJS-C12 stabilized emulsion could significantly enhance oil recovery (∼14.8%), then based on microscopic visualization experiments the potential EOR mechanism was proposed.
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Water
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2023
·Vol. 15
·期 24
·4241
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IF 3.4
Jiamin Chen,Ruijun Ren,Yatao Liu,Chen Li,Zhenbei Wang,Fei Qi
Modification of catalysts by multi-heteroatom doping (S, P, B) is an effective way to improve the peroxomonosulfate activation performance of catalysts. In recent years, highly toxic and persistent trace organic contaminants have been frequently detected in water. Consequently, we proposed the advanced oxidation processes of peroxomonosulfate activated by multi-heteroatom doped Fe@CN (X-Fe@CN) to eliminate trace organic contaminants. The physical phases of X-Fe@CN and its precursors were characterized by X-ray diffraction and scanning electron microscopy. In evaluating the catalytic properties and iron ion leaching of X-Fe@CN-activated PMS for the removal of dicamba and atenolol, B-Fe@CN and PB-Fe@CN were selected and optimized. The active sites of the catalysts were characterized by X-ray photoelectron spectroscopy and Raman. The pathways of PMS activation by B-Fe@CN and PB-Fe@CN were identified in combination with electron paramagnetic resonance and electrochemical experiments. Defects, O-B-O and pyrrolic nitrogen on the surface of B-Fe@CN could adsorb and activate PMS to produce SO4•−, ·OH and1O2. Further doping with P enhanced the electron transfer on the catalyst surface, thus accelerating the activation of peroxomonosulfate. This study compared the effects of multi-heteroatom modifications and further demonstrated the synergistic effect between P and B, which can provide a theoretical basis for the selection of multi-heteroatom doped catalysts in water treatment.Keywords:peroxymonosulfate;trace organic contaminants;multi-heteroatom doping;reaction mechanism
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Journal of Energy Chemistry
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2023
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IF 13.1
Man Yang,Jing Mei,Yujing Ren,Jie Cui,Shuhua Liang,Shaodong Sun
The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance, but still challenging. Herein, we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride (CN). In this Pt 1 -Co 1 /CN bimetallic single-atom catalyst, the noble-metal active sites are maximized, and the single-atomic Co 1 N 4 sites are tuned to Co 1 N 3 sites by photogenerated electrons arising from the introduced single-atomic Pt 1 N 4 sites. Mechanism studies and density functional theory (DFT) calculations reveal that the 3 d orbitals of Co 1 N 3 single sites are filled with unpaired d -electrons, which lead to the improved visible-light response, carrier separation and charge migration for CN photocatalysts. Thereafter, the protons adsorption and activation are promoted. Taking this advantage of long-range electron synergy in bimetallic single atomic sites, the photocatalytic hydrogen evolution activity over Pt 1 -Co 1 /CN achieves 915.8 mmol·g -1 Pt ·h −1 , which is 19.8 times higher than Co 1 /CN and 3.5 times higher to Pt 1 /CN. While this electron-synergistic effect is not so efficient for Pt nanoclusters. These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2019
·Vol. 2019
·期 22
·2761-2767
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IF 2.578
Hongchen Yang,Shengbo Zhang,Mei Li,Xiao Liu,Jinyu Han,Xinli Zhu,Qingfeng Ge,Hua Wang
Graphical Hollow N-doped carbon nanocages incorporating Au and ZnO nanoparticles derived from ZIF-8 were synthesized. Au 0.40 -ZnO/CN incorporates Au and ZnO nanoparticles. Under visible light irradiation, Au 0.40 -ZnO/CN exhibits a significantly enhanced H 2 production rate from formaldehyde alkaline solution, which is 12 times and 2.6 times of those of ZnO/CN and Au/CN, respectively. Hollow carbon nanostructured materials incorporating metals or metal oxides have attracted considerable interest in photocatalysis. Herein, novel hollow N-doped carbon nanocages incorporating Au and ZnO nanoparticles derived from ZIF-8 were successfully synthesized. Firstly, ZIF-8 nanocrystals were treated with chloroauric acid solution (HAuCl 4 ) to produce hollow Au X @ZIF-8 cubes through acid etching of cores and cation exchange. Then, the Au X @ZIF-8 cubes were used as precursors to obtain Au X -ZnO/CN after pyrolysis in a N 2 atmosphere. The resulting Au 0.40 -ZnO/CN had a uniform hollow structure with ≈ 30 nm shells conformal to ZIF-8 dimension while incorporating ≈ 5 nm nanoparticles of Au and ZnO and exhibited remarkable photocatalytic activity and excellent recyclability for hydrogen production from formaldehyde (HCHO) alkaline solution under visible light irradiation. The results demonstrated that incorporation of Au greatly improves the visible light absorption and charge separation via SPR effect. Furthermore, the ZIF-8-derived hollow N-doped carbon cages can expose more uniformly disperse active sites with conductive support. The methodology used here provides a novel approach for preparing hollow hybrid carbon materials with visible-light-driven photocatalytic applications.
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Journal of Water Process Engineering
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2025
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IF 6.7
Yan Shao,Ming Qiao,Jintao Wu,Yifan Yan,Huanhao Chen,Xueying Zhang
This study presents an innovative and eco-friendly method for wastewater treatment, emphasizing the degradation of tetracycline hydrochloride (TCH) through the use of monolithic materials in a trickle-bed dielectric-barrier-discharge (DBD)-based plasma reactor. Modifications to monolithic surface coatings can be utilized to investigate their impact their effects on plasma degradation and energy efficiency. Loading graphitic carbon nitride (g-C 3 N 4 , CN) onto the surface of a monolithic material allows for the modulation of functional groups on the material's surface and the homogeneity of liquid film flow, thereby influencing the generation of active substances and mass transfer at the gas-liquid interface. This study employed hydrothermal techniques to synthesize hydroxyl-grafted and fluorine-grafted g-C 3 N 4 coatings on the surface of open-cell ceramic foam (CN-OH@CF and CN-F@CF, respectively). The CN-OH-6@CF/plasma system exhibits the highest degradation efficiency at 91.1 % and an energy efficiency of 0.5 g/kWh. Active substances generated by plasma, such as ozone (O 3 ), hydroxyl radicals ( OH), and hydrogen peroxide (H 2 O 2 ), were quantified in a liquid falling film DBD-based plasma system. In the CN-OH-6@CF/plasma system, the concentration of OH was 4.55 mg/L at 60 min, the yield H 2 O 2 exceeded 4.04 mg/L and the concentration of O 3 reached 1.17 mmol/L at 60 min. These values were significantly higher than those observed in the CN@CF/plasma or CN-F@CF/plasma systems. The incorporation of – OH groups in CN coatings significantly enhances the production of the direct plasma product O 3 and optimizes O 3 mass transfer at the gas-liquid interface, achieving up to 85 % O 3 contribution in the CN-OH-6@CF/plasma system. The electron transfer number of 2.7 and the H 2 O 2 selectivity of 64.5 % for grafting − F on CN coatings support the selective generation of H 2 O 2 via a two-electron reaction process, as evidenced by rotating ring-disk electrode tests. The selective generation of H 2 O 2 is not conducive to energy efficiency and promotes accelerated degradation. O 3 , in conjunction with H 2 O 2 , promotes the acceleration of its decomposition and the production of OH.
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