Ni single-atom catalysts have been widely explored for CO2 reduction, however, their practical application is often hampered by complex synthesis and instability at high current densities. In this context, well-dispersed nickel nanoparticles present a compelling alternative, offering both facile fabrication and robust performance. Herein, a hierarchical catalyst comprising nickel nanoparticles encapsulated within a nitrogen-doped carbon shell on a hollow-rod carbon substrate (denoted as NiNP-BCN@C) was designed. The hollow-rod architecture maximizes the exposure of nickel nanoparticles as active sites, while the nitrogen-doped carbon shell effectively modulates the electronic environment of the metallic Ni, suppressing the competing hydrogen evolution reaction and promoting CO2 activation. The catalyst exhibits exceptional CO2-to-CO conversion, with a Faradaic efficiency exceeding 90% at −0.83 V vs. RHE in an H-cell and remarkable stability over 32 h. When evaluated in a flow-cell configuration, it achieves a CO Faradaic efficiency > 98% at a current density of 300 mA∙cm−2, corresponding to a high turnover frequency of ~93,579 h−1. In situ Fourier transform infrared spectroscopy revealed intensified bands for key intermediates (*COOH and COO−), confirming enhanced CO2 adsorption and activation. This work showcases a scalable and efficient catalyst design, highlighting the synergy between structural engineering and electronic modulation for advanced CO2 electroreduction.
Polyethylene (PE) plastics pose a severe environmental challenge due to their recalcitrance, which also creates an extremely nutrient-limited environment for microbial colonizers. Understanding the initial adaptive mechanisms is crucial for developing effective bioremediation strategies. In this study, comparative transcriptomics was employed to analyze the specific adaptive response of Bacillus velezensis C5 to PE microplastics by comparing it with responses to a non-polymeric hydrocarbon, n-docosane (C22), and a nutrient-free medium. The results revealed a robust, PE-specific transcriptional program distinct from general starvation or surface-contact responses. Exposure to PE, but not C22, triggered massive upregulation of genes involved in biofilm formation (e.g., the epsA-O operon, including a 185-fold increase in epsL) and sporulation (e.g., a 22-fold increase in yicZ), indicating a polymer-induced strategy for surface colonization and long-term persistence. Although genes associated with canonical PE degradation were not induced, several LLM-class monooxygenases were upregulated, suggesting an auxiliary role in stress mitigation. Phenotypic analyses confirmed that strain C5 remained viable without growth on PE, formed a dense biofilm that increased surface hydrophilicity, and induced only subtle physicochemical changes to the plastic. This study demonstrates that the initial interaction is dominated by a sophisticated, polymer-specific survival program rather than direct metabolic degradation. This insight is fundamental for designing future strategies capable of overcoming this adaptive phase to promote efficient plastic biodegradation.
Complex distillation processes can often be effectively optimized using meta-heuristic algorithms. However, during optimization procedure, a large number of infeasible solutions are generated, hindering efficient exploration of feasible, high-performance regions of the search space. In this study, we propose a data-driven identification and adaptive directed correction strategy for handling infeasible solutions, and on this basis, develop an efficient multi-objective optimization framework (MO-DIDC) for complex distillation processes. By identifying infeasible solutions that closely resemble high-performance ones, the framework leverages them to accelerate convergence to optimal designs. A surrogate model is trained to distinguish high- and low-performance solutions and is then used to identify potentially high-performance candidates within the infeasible set. Through similarity analysis, the most influential variable is selected for correction to generate new promising solutions. This strategy reduces unnecessary exploration of infeasible regions and concentrates computational effort on feasible, high-quality solutions. Demonstrated on a side-stream double-column extractive distillation system and a four-column extractive distillation system, the proposed optimization framework outperforms a widely used genetic algorithm while substantially improving computational efficiency, achieving optimization time reductions of 35.3% and 20.8%, respectively. Overall, the proposed MO-DIDC framework provides an effective and computationally efficient tool for the optimization of complex distillation processes.
Sabatier reaction is an emerging strategy for mitigating anthropogenic CO2 emissions while producing renewable CH4, a versatile energy carrier for heating, electricity generation, and hydrogen production. Developing efficient, low-cost catalysts is challenging, particularly in achieving stable, well-dispersed supports with tunable surface chemistry for methanation. Biochar derived from agrowastes offers a sustainable alternative to conventional oxide supports owing to its low cost, high carbon content, tunable micro-mesoporosity, and ability to anchor metal nanoparticles. Herein, we design and evaluate date palm trunk biochar-immobilized mono and bimetallic Ni, Fe, and NiM (M = Fe or K) catalysts for CO2 methanation. With specific objectives of developing a sustainable supported catalyst by pyrolysis at 500 °C, and evaluating the influence of temperature and pressure on using an industrially relevant H2/CO2 ratio of 3. CO2 methanation performance was assessed in a continuous-flow reactor. The biochar exhibited favorable micro-mesoporous characteristics and high carbon content, enabling effective metal dispersion. Ni loading strongly influenced catalytic performance; the optimal catalyst (0.5 mmol Ni g–1, BCNi-3.0) achieved 58% CO2 conversion and 91% CH4 selectivity at 400 °C and 1 bar. Increasing pressure to 30 bar enhanced performance to 76% CO2 conversion and nearly 99% CH4 selectivity, with stable operation over 20 h. Bimetallic NiFe catalysts formed NiFe2O4 and NiO phases and promoted CO formation via the reverse water gas shift reaction, while K promotion further favored CO production. Overall, biochar-supported Ni-based catalysts demonstrate a sustainable and efficient platform for CO2 methanation with reduced hydrogen demand.
Cerium oxide (CeO2) is a critical abrasive in chemical mechanical polishing (CMP) due to its chemical-mechanical reactivity and planarization capability. This study developed a controllable hydrothermal synthesis strategy for spherical CeO2 abrasives and systematically evaluated their CMP performance on silicon wafers. Uniform CeO2 particles with a fluorite structure were synthesized, as confirmed by scanning electron microscopy, X-ray diffraction, and high-resolution transmission electron microscopy analyses. Mechanistic studies reveal that CeO2 formation occurred via nitrate-induced oxidation of Ce3+. The subsequent precipitation of CeO2, coupled with acetate decomposition, thermodynamically drove the reaction forward under hydrothermal conditions. By adjusting water volume, the particle size was precisely tuned from 32 to 531 nm while maintaining excellent sphericity and dispersity. CMP tests showed that 343 nm CeO2 achieved the highest material removal rate (73.7 nm∙min–1) with low surface roughness (Ra = 0.31 nm). Optimal polishing with 0.5 wt% CeO2 achieved a balance between removal efficiency and surface quality, while higher concentrations led to residue defects. Moreover, the hydrothermally synthesized CeO2 exhibited better CMP performance than commercial abrasives in both short- and long-term polishing, owing to its uniform morphology. Overall, this work demonstrates a simple, effective, and scalable strategy for synthesizing size-controlled CeO2 abrasives with excellent performance in precision surface processing.
Antibiotics have revolutionized infectious disease management; however, their incomplete absorption and metabolism by humans lead to environmental discharge, posing severe threats to ecosystems. Levofloxacin (LEV), a typical broad-spectrum fluoroquinolone antibiotic, is highly resistant to microbial biodegradation in aqueous environments and poses a major threat to human health and ecological systems. This paper presents a facile and robust strategy for fabricating Zn1−xCuxS nanoparticle (NP)-decorated cellulose–chitosan composite sponges (denoted as ZnCuCCS). The synthetic route integrates hydrothermal xanthate decomposition and in situ deposition, producing a porous composite characterized by homogeneous Zn1−xCuxS NPs dispersion, strong Nanoparticle anchoring, and superior mechanical stability. Benefiting from the abundant adsorption sites provided by the polysaccharide sponge matrix and the high surface exposure of Zn1−xCuxS NPs, ZnCuCCS possesses a narrow bandgap (1.31 eV), which endows the composite with superior adsorption capability and prominent photocatalytic activity, achieving a LEV removal efficiency of up to 90.12%. Notably, ZnCuCCS maintains a stable degradation rate of 72.9% even after five consecutive reuse cycles. Systematic investigations of the adsorption–photocatalytic degradation behavior and intrinsic mechanism of LEV removal provide novel theoretical insights for the rational design and practical application of advanced photocatalytic materials in wastewater treatment.
CO2 hydrogenation coupled with toluene alkylation is a promising route for application in greenhouse gas utilization and para-xylene (PX) production; however, the strong Brønsted acid sites of the conventional ZSM-5 catalyst lead to uncontrollable (de)alkylation and xylene isomerization. In this study, a silanol nest-enriched silicalite-1 zeolite (AS-1) with a moderate acidity was employed as an alkylation catalyst to suppress side reactions. Dealkylation and xylene isomerization were significantly suppressed compared to those observed using ZSM-5, which reduced the benzene selectivity from 6.04% to 0.5% and increased the PX selectivity from 23.6% to 33%. An epitaxial silicalite-1 shell was introduced to passivate the external sites to enhance the shape-selective effect of AS-1, thus improving the PX selectivity from 36.2% to 44.4%. The intimate contact established by optimizing the spatial distribution facilitated the conversion of the methanol intermediates, increasing the toluene conversion to 16.3%. A deposition-precipitation strategy was adopted to load ZnZrOx particles onto silicalite-1 zeolite-coated AS-1, which increased the ZnZrOx dispersion and minimized the transfer distance for the methanol intermediates. Consequently, considerable levels of toluene conversion and a high PX selectivity of 15% and 42.7%, respectively, were maintained, while the CO2 conversion significantly increased from 5.9% to 9.5%. Additionally, ammonium hexafluorosilicate treatment generated small mesopores within the AS-1 zeolite, which enhanced diffusion and further increased the toluene conversion to 20.9%. This study provides novel insights into the design of bifunctional catalysts comprising silanol nest-enriched silicalite-1 and ZnZrOx for use in CO2 hydrogenation coupled with toluene alkylation.