The development of low-cost, green, and environmentally friendly capacitive deionization (CDI) electrodes for seawater desalination remains a challenging task. In this study, tea-residue waste was employed as a carbon precursor to fabricate a hierarchical porous carbon electrode via a green and low-corrosivity strategy involving K2CO3 impregnation activation followed by one-step carbonization. The desalination performance of the obtained materials was comprehensively evaluated. Electrochemical measurements revealed that TKC(0.09)-800 delivered a specific capacitance of 142.6 F g- 1 at a current density of 0.5 A g-1. Under an applied voltage of 1.2 V, a flow rate of 10 mL min- 1, and an initial salt concentration of 600 mg L- 1, it attained a salt adsorption capacity of 25.38 mg g- 1 with a maximum salt adsorption rate of 12.14 mg g- 1 min- 1. This work offers a sustainable strategy for fabricating biomass-based porous carbon electrodes for CDI applications.
Abstract The practical use of nickel catalysts is severely limited by surface oxidation, which passivates active sites with a NiO layer, resulting in a debilitating induction period. While protective strategies exist, they inevitably compromise the accessibility and intrinsic activity of Ni sites. Herein, we introduce a paradigm shift from static protection to dynamic self-healing via hydrogen spillover in a Ni-Pd/CeO2 architecture. Trace Pd (0.2 wt %) acts as efficient hydrogen-dissociation centers, from which active hydrogen species migrate via the CeO2 support to continuously reduce the passivating NiO layer in situ. This process dynamically exposes metallic Ni0 sites under operation, which function as the primary centers for furan ring activation. In contrast to the conventional Ni/CeO2 catalyst, which suffers from a debilitating induction period, the Ni-Pd/CeO2 system achieves an activity enhancement of 55-fold in TOF for the hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol. Combined spectroscopic and kinetic experiments, including H2-TPR, H−D exchange, Pd loading optimization, and support effect studies, corroborate the hydrogen spillover mechanism. This work represents a paradigm shift from conventional static protection strategies to dynamic self-healing mechanisms, establishing a general blueprint for designing self-sustaining non-precious metal catalysts, paving the way for their use in cost-efficient catalytic processes.
Supercapacitor performance is largely determined by electrode materials. Transition metal compounds (TMCs) have high theoretical capacities but suffer from sluggish charge transport and volume-induced structural degradation, which limits their practical applications in energy storage. To overcome the inherent bottlenecks of TMCs in energy storage, this work reports a novel dual-regulation strategy to construct a P-doped CoO/Co9S8 heterostructure anchored on activated carbon (P-CoO/Co9S8@AC). The formation of the P-doped CoO/Co9S8@AC heterostructure enables close coupling between macroscopic structural buffering and atomic-scale electronic modulation. Introducing activated carbon (AC) suppresses particle agglomeration and buffers volume expansion, while the synergistic effect of heterointerface engineering and P doping significantly reduces the charge-transfer resistance to 0.27 Ω. Benefiting from these multidimensional advantages, the as-prepared material delivers a specific capacity of 1697.3 C g-1 (3394.6 F g-1) at 1 A g-1, outperforming previously reported nickel sulfide/nickel oxide heterostructures (2278 F g-1) and P-doped ternary cobalt-based sulfide electrodes (2716 F g-1). Density functional theory (DFT) calculations show that the P-doped heterostructure has an OH- adsorption energy of -4.82 eV and an upshifted d-band center, thereby improving intrinsic conductivity and OH- interfacial adsorption. Furthermore, the assembled hybrid supercapacitor (HSC) achieves a high energy density of 90.4 Wh kg-1 at a power density of 750 W kg-1, while retaining 86.1% of its capacity after 20,000 cycles. This study provides a design strategy for constructing high-performance composite electrodes by integrating heterointerface engineering and heteroatom doping.
5-Methoxymethyl-2-furfural (MMF) serves as a crucial biobased platform molecule that can be transformed into various high-value chemicals and biobased polyester monomers. However, the current production of MMF still faces several challenges, such as low yield and prolonged reaction time. In this study, we prepared a series of amide-modified strongly acidic resin catalysts and discovered that they have a higher efficiency in converting fructose to prepare MMF in 1-Butyl-3-methylimidazolium chloride ([BMIM]Cl) and methanol. Among the synthesized catalysts, DB757-NMP demonstrated superior performance, achieving an MMF yield of approximately 61.5% under the optimized conditions, with a combined yield of HMF and MMF reaching about 66.6%. The catalyst formation mechanism was analyzed using FTIR, and NMR, confirming the transformation of proton between NMP and the sulfonic acid groups of the resin, which collectively promoted the conversion of fructose to MMF. In addition, we investigated main reasons for catalyst deactivation and successfully restored catalytic activity through regeneration. The regenerated catalyst could be reused for three times with only a slight decrease in MMF yield. The results suggested that DB757-NMP is a more sufficient and recyclable catalyst for the production of MMF from fructose. This work presented a simple and environmentally benign approach for the synthesis of MMF.
Biomass-derived materials offer renewability and waste valorization for water purification, yet identifying and controlling their precise ROS-driven degradation pathway in peroxymonosulfate (PMS)-based systems remains a fundamental challenge. Herein, we report N-doped cobalt-carbon catalysts (Co-CN-X) from cotton via polymerization-pyrolysis and show how nitrogen doping tailors PMS activation for pollutant degradation. Upon nitrogen introduction, the optimized Co-CN-24 catalyst achieves efficient carbamazepine degradation, reaching 96.55% within 35 min with a 7.12-fold enhancement in reaction efficiency compared to the Co-C counterpart. Integrated characterization and DFT calculations reveal that Co-CN-24 possessing high pyrrolic N and Co0 content abundant facilitates 1O2 generation, thereby increasing the dominance of non-radical pathways in pollutant degradation. Most importantly, the Co-CN-24/PMS system exhibits selective reactivity toward electron-rich pollutants, broad pH tolerance, and robust performance in complex water matrices, including continuous flow experiments. This work provides mechanistic insight into how nitrogen doping regulates non-radical pathways in biomass-derived catalysts, offering a sustainable strategy for targeted pollutant remediation.
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have emerged as a promising strategy for the efficient removal of organic contaminants from wastewater. Catalyst plays a crucial role in PMS activation within AOPs. However, many catalysts suffer from deactivation due to metal ion leaching and this is also the main cause of secondary pollution. Perovskite oxides demonstrate excellent stability and high efficiency in AOPs. In this study, a novel perovskite oxide Sr0.8Ca0.2Co0.6Fe0.4O3-delta (SCCF) was synthesized by partially substituting Sr with Ca at the A-site of SrCo0.6Fe0.4O3-delta (SCF). SCCF shows outstanding stability, as evidenced by its strong resistance to impurities, acid-base tolerance, and cycling stability. Furthermore, SCCF demonstrated exceptional long-term performance under continuous-flow operation for over 600 h with even negligible metal leaching. In Norfloxacin (NOR) degradation, SCCF achieved a removal efficiency of 94.8 % within 15 min. Mechanistic studies identified four dominant reactive oxygen species (ROS)-hydroxyl radicals (center dot OH), sulfate radicals (SO4 center dot-), singlet oxygen (1O2), and superoxide radicals (O2 center dot-)-contributing synergistically to the degradation process. The DFT analysis reveals that Ca doping at the A-site not only increases oxygen vacancy concentration but also modulates the electronic distribution around Co and Fe sites, which enhances PMS activation and active species generation. This work offers insights into rational perovskite design for highly stable and efficient AOP catalysts in practical water treatment applications.
In recent years, the integration of two-dimensional MXenes with transition metal compounds (TMOs, LDHs, TMDs) has attracted considerable attention as an effective strategy for developing high-performance flexible supercapacitors. This review systematically examines advances from the past decade in the rational design, synthesis, and application of MXene/transition metal compound hybrids. We highlight how transition metal compounds serve as spacers to mitigate MXene restacking while contributing abundant redox-active sites, and how MXenes provide conductive networks that enhance charge transfer kinetics. The interplay between these components leads to exceptional electrochemical performance, including high capacitance, energy density, and cycling stability in flexible devices. By critically analyzing synthesis strategies, interfacial interactions, and material properties, this review offers new insights into the synergistic mechanisms and provides guidelines for the future development of MXene-based composites towards practical wearable energy storage.
Zinc-ion hybrid capacitors (ZIHCs) have emerged as a promising energy storage technology, integrating the merits of high-power supercapacitors and high-energy batteries while offering cost-effectiveness and safety. However, their commercialization is hampered by challenges such as limited energy density, low power output, and poor cycling stability. Herein, we report a sustainable strategy to fabricate heteroatom-doped coral-like hierarchical porous carbon (LCK-800) as an advanced cathode for ZIHCs. The synthesis of LCK-800 synergistically utilizes industrial sodium lignosulfonate and chitosan through hydrogen-bond-directed self-assembly. This approach generates a 3D interconnected meso/microporous architecture and large surface area measuring 2227.32 m2 g-1 along with adjustable heteroatom doping capabilities. Assembled as a ZIHC with a Zn anode in 2 M ZnSO4 electrolyte, LCK-800 exhibits remarkable performance: a gravimetric capacitance reaching 202 mA h g-1 under 0.1 A g-1 current density, an energy density of 189 W h kg-1 at a power density of 97 W kg-1, and preserving 97.5 % of its original capacity through 10,000 operational cycles under 5 A g-1. This study not only provides a green, template-free approach for synthesizing high-performance heteroatom-doped carbons but also offers insights into the structure-property relationships of ZIHCs, facilitating the advancement of novel ecofriendly energy storage systems for future applications.
The construction of porous carbon materials while minimizing the use of chemical activating agents remains a considerable challenge. In this work, kelp, a renewable and environmentally friendly biomass, was employed as the carbon source to fabricate porous carbon for supercapacitor applications. Taking advantage of the excellent hygroscopicity of kelp, a trace amount of sodium bicarbonate, two orders of magnitude lower than that used in conventional methods, was utilized as the activating agent to produce porous carbon with a high specific surface area. Compared with the unactivated sample, the obtained sample after the activation exhibited a well-developed porous structure and outstanding electrochemical performance. In a three-electrode configuration, the optimized sample KCX (0.02)-700 delivered a high specific capacitance of 442.75 F g- 1 at a current density of 0.5 A g- 1. When assembled into a symmetric electric double-layer capacitor, its energy density reached 38.23 Wh kg- 1 at a power density of 250 W kg-1. After 10,000 charge-discharge cycles, 95.10% of its initial capacitance was retained. Furthermore, the samples fabricated using the proposed strategy displayed notably improved electrochemical performance when compared with those prepared through the traditional post-carbonization activation process. This study indicates that KCX is a sustainable and high-performance biomass-derived carbon material, which holds considerable potential for applications in next-generation energy storage devices.
Zn||MnO2 batteries operated at elevated temperatures often undergo changes in the local water microenvironment of electrolytes, accompanied by intensified parasitic reactions and reduced stability of the Zn anode and MnO2 cathode. Herein, a bio-derived hydrogel electrolyte is prepared from locust bean gum and acrylamide through hydrogen-bond regulation. During polymerization, hydroxyl-rich locust bean gum interacts with the resulting polyacrylamide network through hydrogen bonding and chain entanglement, contributing to water retention and continuous pathways for hydrated Zn2+ transport. FTIR and Raman analyses reveal a redistribution of the hydrogen-bonding environment, indicating reorganization of polymer–water interactions within the LAG network. This regulated water microenvironment reduces thermally induced water loss while maintaining sufficient molecular mobility for hydrated Zn2+ transport. The LAG hydrogel electrolyte exhibits an apparent Zn2+ transference number of 0.73, an ion-transport activation energy of 7.4 kJ mol-1, and improved mass retention at 60 °C. These characteristics are associated with moderated interfacial pH variation, reduced Zn corrosion and by-product accumulation, and lower Mn dissolution and cathode deterioration during cycling. At 60 °C, Zn||Ti cells deliver an average Coulombic efficiency of 98% over 130 cycles, Zn||Zn symmetric cells operate for more than 300 h, and Zn||MnO2 full cells retain 90.1% of their initial capacity after 1000 cycles at 2 A g-1. This work presents a hydrogen-bond-regulation approach for coupled electrode stabilization in Zn||MnO2 batteries under elevated-temperature conditions.
Spent coffee grounds (SCG) have been serving as a widely available and low-cost source of lignocellulosic biomass resource for fabricating value-added functional materials for wastewater treatment. Nevertheless, the surface of raw SCG lacks sufficient active cationic adsorption sites, resulting in limited adsorption capacity for anionic dyes. To construct highly efficient and functional amine-rich adsorption sites, this study utilized SCG as an amine-rich adsorbent for the removal of methyl orange (MO) through a process involving gradient delignification followed with grafting of polyethyleneimine (PEI) of varying molecular weights. The delignification degree regulated the balance between structural opening and framework preservation, while PEI molecular weight determined grafting efficiency and amino-site accessibility. Moderate delignification produced an optimized SCG-D1 substrate with an exposed cellulose-enriched framework, improved pore accessibility and sufficient structural integrity. Low-molecular-weight PEI was more effectively immobilized on SCG-D1 than medium- and high-molecular-weight PEI, while the moderately delignified SCG-D1 framework further promoted the accessibility and utilization efficiency of the introduced amino sites. Consequently, SCG-D1-L exhibited the best MO adsorption capacity, 308.55 mg/g. Substrate-dependent verification using different delignified SCG substrates grafted with the same low-molecular-weight PEI further confirmed SCG-D1 as the optimal functionalization platform, as it enabled the formation of a more available amino-rich adsorption interface. This work provides useful guidance for designing biomass-derived adsorbents through coordinated regulation of substrate structure and functional-site accessibility.
Aqueous zinc-ion batteries (AZIBs) have important application prospects in the field of high-temperature energy storage. However, traditional aqueous electrolytes have high ionic conductivity, but they are challenged by hydrogen evolution reactions and imbalanced of zinc-ion transference number. To address this issue, we used acrylamide guar gum as the skeleton and introduced potassium 3-sulfonate propyl methacrylate (SPMAK), through the Hofmeister effect. On the one hand, sulfonic acid groups form strong coordination with zinc-ion, reconstructing the solvation sheath of hydrated zinc-ion and replacing some active water molecules, significantly reducing the desolvation energy barrier, while reconstructing the hydrogen bond network, inhibiting proton conduction and hydrogen evolution side reactions. On the other hand, SPMAK can construct highly ordered sulfonic end nanochannels on the electrode surface, forming zinc-ion selective transport channels, increasing the zinc-ion transference number to around 0.68, and achieving uniform distribution of ion flux. This further solves the problems of low and uneven distribution of hydrogen evolution reaction and zinc-ion transport efficiency at high temperatures. At 60 ℃, the coulomb efficiency of AKG-Z gel electrolyte reached 99.02% after 370 cycles. Under the conditions of 60 ℃ and 1 A g−1, the capacity retention rate of Zn || AKG-Z || MnO2 batteries remained as high as 95.1% after 1500 cycles, demonstrating excellent high-temperature long cycle stability.
Aqueous Zn||MnO2 batteries suffer instability at elevated temperatures due to a coupled degradation involving free water activation, Mn dissolution/shuttling, and parasitic interfacial reactions. Here, we propose a solvationgoverned shuttle suppression strategy using a pectin/acrylamide composite hydrogel electrolyte (PAG). The abundant-COO--/--OH groups in pectin restructure the hydrogen bond network, promoting the formation of a confined/bound-water environment and reshaping the Zn2+ solvation environment. This suppresses free-water-assisted Mn dissolution and Mn2+ shuttling, which are linked to pseudocapacitive currents and interfacial instability. As a result, the electrochemical process shifts from shuttle-affected, capacitive-dominated behavior toward diffusion-controlled Zn2+ insertion/extraction. The stabilized solvation also mitigates Zn corrosion, hydrogen evolution, and interfacial fluctuations. Consequently, PAG-based Zn||MnO2 cells retain about 83% capacity after 1000 cycles at 1 A g-- 1 and about 90% after 1500 cycles at 2 A g-- 1 at 60 degrees C. This work reveals that Mn shuttling is a solvation-governed electrochemical instability and provides a general electrolyte design principle for high-temperature aqueous batteries.
Biomass resources, characterized by their wide distribution, carbon neutrality, and renewability, have emerged as ideal alternatives to fossil fuels. Derived from these resources, bio-based platform compounds such as 5-hydroxymethylfur- fural (HMF) and 2,5-diformylfuran (DFF) exhibit diverse application potential. These bio-based platform compounds can be converted into high-value-added chemicals through organic chemical reactions. Bio-based polyacid esters show broad potential for applications in fields such as chemical engineering, polymer materials, and biomedicine, where they can serve as crosslinking agents, lubricants, emulsifiers, among other roles. Conventional methods for synthesizing polybasic acid esters typically involve strong oxidants, intricate processes, and demanding equipment requirements. In this study, we prepared a series of supported ionic liquid catalysts via in-situ acid-base neutralization reaction, employing weak acidic ion exchange resin as the solid support and organic amines as functional modifiers, and used them to the preparation of bio-based polyacid esters. When 2,5-diformylfuran (DFF) and dimethyl malonate (DMM) were employed as substrates, the yield of bio-based polyacid esters can reach 99.2% in the presence of Pyrrolidine-YLST-3. The structural modifications of the resins were comprehensively characterized using multiple analytical techniques, including elemental analysis (EA), nuclear magnetic resonance (NMR), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). These comprehensive analyses provided conclusive evidence for the successful surface modification of YLST-3 resin with pyrrolidine, revealing distinct chemical interactions between the modifier and the resin. Comprehensive characterization of both fresh and deactivated catalysts was performed using EA, FTIR, and XRD to investigate catalyst deactivation mechanisms. Successful regeneration was accomplished through a two-step protocol involving hydrogen peroxide oxidation followed by pyrrolidine re-modification, which substantially improved cycling stability. Substrate scope evaluation demonstrated that the Pyrrolidine-YLST-3 catalyst exhibited excellent activity in Knoevenagel condensation reactions across diverse substrates, confirming its broad applicability.
The properties of biomass-derived multifunctional materials have garnered increasing attention in the fields of environmental remediation, energy storage, and heterogeneous catalysis due to their abundant content of N and C, which can effectively modulate electronic structure and facilitate the anchoring of active centers. In this review, we summarized the progress of our team over the past decade on a variety of multifunctional materials with diverse morphologies, electronic structures, and geometric sites, developed through novel synthetic strategies that employ biomass and its derivatives as carbon sources. Those multifunctional materials exhibited excellent catalytic performance for the adsorption and degradation of pollutants in wastewater, absorption of electromagnetic waves (EMW), and photocatalytic reactions. Moreover, the underlying mechanisms of adsorption, degradation, and activation during the reaction process as well as the relationship between activity and structure are also discussed. This review offers comprehensive insights for fabricating biomass-derived materials, with a specific emphasis on their physicochemical properties characterized by controlled morphology, tunable electronic properties, and precise localization of active species, as well as the aspect of the intricate relationship between activity-structure and catalytic mechanisms, providing reference for future advancements in various catalysis fields involving biomass-derived materials. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
The recovery of gold from secondary resources is of considerable socio-economic and environmental importance.
Methylene blue (MB) is a typical cationic dye characterized by significant stability and poor degradability, posing a potential risk to the environment. In this study, spent coffee grounds (SCG) were modified using NaOH treatment to prepare biomass-derived adsorbents (NaOH-SCG) for MB removal, and the preparation conditions were optimized with response surface methodology (RSM). NaOH concentration and treatment time were considered to be key factors influencing the interfacial properties and adsorption performance of SCG. The study showed that moderate NaOH treatment induced interfacial reconstruction of SCG by disrupting the dense lignocellulosic structure, exposing oxygen-containing groups, enhancing surface negative charge and improving pore accessibility. Among these, the 10 wt%-12h sample exhibited the best adsorption performance, reflecting a good balance had been achieved between the degree of surface activation and framework preservation. The adsorption behavior was more accurately described by the PSO kinetic and Langmuir isotherm models, with the Langmuir-derived maximum adsorption capacity of 407.08 mg/g at 25 °C. Weber-Morris and Boyd analyses indicated that MB uptake involved rapid surface adsorption, boundary-layer diffusion and pore-assisted diffusion rather than a single diffusion-controlled step. After six adsorption-desorption cycles, the 10 wt%-12h sample still maintained considerable adsorption capacity and removal efficiency. The FTIR and XPS confirmed the formation of an MB-rich adsorption layer and the involvement of -OH, CO, C-O and N-containing surface species. Overall, MB adsorption was mainly driven by electrostatic attraction, assisted by hydrogen bonding, polar interactions, possible π-π interactions and pore-assisted diffusion.
The practical application of aqueous zinc-ion batteries (AZIBs) is significantly hindered by the unregulated growth of dendrites and the instability at the interface of Zn anodes. Here, we report an interfacial engineering strategy using ionic liquid modified electrolytes to achieve uniform Zn deposition and long-term stability. Two imidazolium-based ionic liquids, 1-butyl-3-methylimidazolium chloride (BmCl) and 1-butyl-3-methylimidazolium bromide (BmBr), were incorporated to regulate Zn2+ solvation structure and interfacial behavior. The imidazolium cation (Bm+) exhibits preferential adsorption on the Zn(002) facet, forming a compact protective layer, while halide anions (Cl-/Br-) tune Zn2+ desolvation and migration kinetics. Combined spectroscopic and theoretical analyses reveal that BmBr possesses a higher desolvation energy and stronger interfacial regulation capability, which effectively promote selective Zn(002) oriented growth and suppress dendrite formation. As a result, Zn||Zn symmetric cells using the BmBr/ZnSO4 (BmBr/ZSO) electrolyte demonstrate exceptional cycling stability, maintaining performance for over 5000 h at 0.5 mA cm-2 and 0.5 mAh cm-2. Furthermore, Zn||NVO full cells exhibit a remarkable specific capacity of 401 mAh g-1 at 0.1 A g-1, along with excellent cycling stability. The BmBr/ZSO electrolyte also effectively suppresses self-discharge. This study elucidates the underlying mechanisms of cation-anion driven regulation and presents a broadly applicable approach for developing high-performance, dendrite-free AZIBs.
The hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL) represents a critical route for biomass valorization, yet catalyst deactivation remains a major challenge. Herein, we engineer metal-support interaction (MSI) in ceria-supported cobalt catalysts (xCoCe) by tuning the cobalt loadings (0.5-5 wt%) to achieve durable and efficient LA upgrading. The optimized 1CoCe catalyst exhibits 100% yield of GVL and a stability of 900 h in continuous operation, surpassing the performance of reported non-precious metal catalysts. Investigations, including XPS, Raman spectroscopy, and H2-TPR, reveal that 1CoCe possesses higher contents of both Co2+ and oxygen vacancies, which enhance the MSI effects that guarantee catalyst stability. This study highlights MSI modulation as a versatile strategy for designing non-precious metal catalysts and advancing scalable and sustainable biomass conversion technologies.
The interfacial incompatibility between inorganic metal oxides and polymers severely limits the utilization of hybrid cathodes in aqueous zinc-ion batteries (AZIBs). Herein, we propose a Cu2+ ion mediated interfacial reinforcement strategy guided by the hard-soft acid-base principle to strengthen the interaction between alpha-MoO3 and polyaniline (PANI). The introduced borderline acidic Cu2+ ions on the alpha-MoO3 surface provides effective anchoring sites for PANI through strong Cu-N coordination, which accelerates the in-situ growth of PANI, suppresses polymer self-aggregation, thus enabling a uniform coating on MoO3 nanorods. In addition, Cu2+ incorporation selectively promotes the exposure of MoO3 facets that are thermodynamically favorable for PANI adsorption, further enhancing interfacial compatibility. As such, the PANI loading is increased by 66.79%, forming a conformal shell structure on MoO3. The hybrid cathode exhibits suppressed proton penetration, mitigated parasitic reactions, accelerated zinc ion transport kinetics, and robust structural integrity. Consequently, the cathode delivers a high specific capacity of 397.20 mAh g- 1 at 0.2 A g- 1 and maintains 278.35 mAh g- 1 even at 10 A g- 1. After 5000 cycles at 5.0 A g- 1, it retains 98.95% of its initial capacity with Coulombic efficiency approaching unity (similar to 100%) in AZIBs. This work provides a general interfacial engineering strategy for constructing high performance hybrid electrodes.