APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Xinzheng Ma,Jingyi Chen,Ziang Zhao,Ronghe Lin,Xiaoling Mou,Yihui Li,Li Yan,Hejun Zhu,Yunjie Ding
Solvent-free oxidation of benzyl alcohol on bimetallic Pt-Bi catalysts supported on activated carbon (AC), carbon black, carbon nanotube, and N-doped carbon (NC) was studied. While the dispersions of both metals significantly increased on all the bimetallic catalysts, the composition and distribution of the metal species were strongly influenced by different supports. The formation of PtBi alloy was favored on most supports except AC, where aggregation of Bi was observed. Moreover, the oxidation activity was found to closely link to the surface Bi:Pt ratios. Extensive optimizations on PtBi/NC catalyst in batch and flow reactors yielded impressive benzaldehyde yields of 86 % and 70 %, respectively, under mild conditions, which are comparable or even superior to the performances of most state-of-the-art catalysts. Notably, a 96-hour continuous test in a trickle-bed reactor demonstrated stable operation without catalyst deactivation, demonstrating the promising industrial potential.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-15
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IF 14.7
Cui Lele,Chen Bin,Chen Dongxu,He Chen,Liu Yi,Zhang Hongyi,Qiu Jian,Liu Le,Jing Wenheng,Zhang Zhenghua
The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H 2 O 2 electrosynthesis community. However, it remains perplexing that electrocatalysts and assembled GDE frequently exhibit substantial discrepancies in H 2 O 2 selectivity during bulk electrolysis. Here, we elucidate the pivotal role of mass transfer behavior of key species (including reactants and products) beyond the intrinsic properties of the electrocatalyst in dictating electrode-scale H 2 O 2 selectivity. This tendency becomes more pronounced in high reaction rate (current density) regimes where transport limitations are intensified. By utilizing diffusion-related parameters (DRP) of GDEs (i.e., wettability and catalyst layer thickness) as probe factors, we employ both short- and long-term electrolysis in conjunction with in-situ electrochemical reflection-absorption imaging and theoretical calculations to thoroughly investigate the impact of DRP and DRP-controlled local microenvironments on O 2 and H 2 O 2 mass transfer. The mechanistic origins of diffusion-dependent conversion selectivity at the electrode scale are unveiled accordingly. The fundamental insights gained from this study underscore the necessity of architectural innovations for mainstream hydrophobic GDEs that can synchronously optimize mass transfer of reactants and products, paving the way for next-generation GDEs in gas-consuming electroreduction scenarios.
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Small
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2024
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IF 13
Tong Hu,Shufen Zhang,Yong Qi
The ability to reversibly exhibit structural color patterns has positioned photonic crystals (PCs) at the forefront of anti-counterfeiting. However, the security offered by the mere reversible display is susceptible to illicit alteration and disclosure. Herein, inspired by the electronic message captcha, bilayer photonic crystal (BPC) systems with integrated decryption and verification modules, are realized by combining inverse opal (IO) and double inverse opal (DIO) with polyacrylate polymers. When the informationized BPC is immersed in ethanol or water, the DIO layer displayed encrypted information due to the solvent-induced ordered rearrangement of polystyrene (PS) microspheres. The verification step is established based on the different structural colors of the IO layer pattern, which result from the deformation or recovery of the macroporous skeleton induced by solvent evaporation. Moreover, through the evaporation-induced random self-assembly of PS@SiO 2 and SiO 2 microspheres, unclonable structurally colored identifying codes are created in the IO layer, ensuring the uniqueness upon the verification. The decrypted code in the DIO layer is valid only when the IO layer displays the pattern with the predetermined structural color; otherwise, it is a pseudo-code. This structural color-based “decryption-verification” approach offers innovative anti-counterfeiting applications in nanophotonics.
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Journal of Energy Storage
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2024
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IF 8.9
Hanbo Wang,Dongyu Pei,Yiduo Li,Ziqi Zhang,Sheng Wan,Ziming Wang,Mingrui Yu,Haiyan Lu
It has been generally accepted that the negative electrode of aqueous nickel‑carbon asymmetric capacitors underwent capacitive reactions. However, through further research, we have unveiled an additional electrochemical reaction occurring on the negative electrode. Nickel ions were reduced to nickle and deposited on the surface of the negative electrode, which subsequently transformed to nickel oxides. This previously unrecognized phenomenon significantly impacted the energy density and cycle life of nickel‑carbon supercapacitors . The introduction of anion exchange membranes between the positive and negative electrodes was demonstrated as an effective solution in inhibiting the uncontrolled diffusion of nickel ions onto the surface of the negative electrodes. This modification led to a remarkable increase in capacity retention rate of the alkaline nickel‑carbon supercapacitor , rising from 70.45 % to 97.76 % after 10,000 cycles. Furthermore, the modified supercapacitor continued to operate reliably for over 45,000 cycles, extending the cycle life by nearly fivefold. The suppression of nickel deposition on the negative electrode represented a critical advancement in enhancing the performance and lifespan of nickel‑carbon supercapacitors.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Hong-Yu Wang,Shi-Lin Mei,Xiao-Lan Tan,Bao-Hua Lu,Nan Li,Zhen-Bo Wang
The commercialized lithium nickel manganese cobalt oxides have been extensively applied for high-rate lithium-ion batteries due to its collective merits of fast kinetics, high specific capacity, and reasonable cost. The optimization on lithium nickel manganese cobalt oxide particles is crucial for high-rate batteries since the rate capability, storage and cycling stability are highly dependent on the chemical and physical properties of the cathode materials. Herein, the particle-feature influence on the high-rate performances is investigated to unveil the structure-property relationship. Through systematic electrochemical analysis and material characterizations, a direct comparison among commercial lithium nickel manganese cobalt oxide cathode materials with different particle size, doping, and crystalline structures has been performed. It is found that for polycrystalline lithium nickel manganese cobalt oxide materials, appropriate Al and Zr doping and small particle size are beneficial to superior rate performance and cycling stability up to 30 C. While single-crystalline particles show outstanding storage properties compared to polycrystalline particles with similar size and ion doping. Morphological and structural evolution of the lithium nickel manganese cobalt oxide particles after cycling has been revealed including the changed mixing degree of Li + /Ni 2+ , collapsing of primary particles and different parasitic reactions between the electrolyte and the particle surface. This work can provide direct guidance for the subtle design of efficient cathodes for high-rate lithium-ion batteries.
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ADVANCED MATERIALS
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2025
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IF 26.8
Lei Zhuang,Zihao Wen,Yiwen Liu,Jing Yang,Hulei Yu,Yanhui Chu
Understanding the behavior of high-entropy carbides (HECs) under oxygen-containing environments is of particular importance for their promising applications in structural components, catalysis, and energy-related fields. Herein, the structural evolution of (Ta, Ti, Cr, Nb)C (HEC-1) nanoparticles (NPs) is tracked in situ during the oxidation at the atomic scale by using an open-cell environmental aberration-corrected scanning transmission electron microscope. Three key stages are clearly discerned during the oxidation of HEC-1 NPs at the atomic level below 900 °C: i) increased amorphization of HEC-1 NPs from 300 to 500 °C due to the energetically favorable formation of carbon vacancies and substitution of carbon with oxygen atoms; ii) nucleation and subsequent growth of locally ordered nanocluster intermediates within the generated amorphous oxides from 500 to 800 °C; and iii) final one-step crystallization of non-equimolar MeO 2 and Me 2 O 5 (Me = metallic elements, Ta, Ti, Cr, and Nb) high-entropy oxides above 800 °C, accompanied with the reduction in atomic defects. This result is further confirmed by theoretical calculations that these observed high-entropy oxide phases are thermodynamically preferable to generate above 830 °C. The study provides direct evidence of the ordered–disordered–ordered structural transition of HECs during oxidation.
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DESALINATION
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2025
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IF 9.8
Jundong Zhao,Shui Liu,Qingyu Lai,Lele Liu,Yunan Gao
Cationic dyeing wastewater poses severe environmental threats by releasing persistent aromatic dyes that suppress aquatic photosynthesis, accumulate in soil to inhibit plant growth, and generate carcinogenic byproducts through photodegradation or chlorination, thereby disrupting ecosystem stability. Carboxylated graphene oxide/sodium alginate-activated carbon aerogel spheres (CGO-AC/SA) were engineered to address cationic dye pollution through a synergistic integration of tailored carboxylation, hierarchical porosity, and DFT-guided mechanistic insights. The composite achieved unprecedented adsorption capacities of 650.695, 546.471, and 385.634 mg/g for methyl violet (MV), methylene blue (MB), and basic fuchsin (BF), respectively. Multi-scale analyses revealed that carboxylation amplified surface charge density ( COO − ) and enabled selective electrostatic interactions with cationic dyes, while hierarchical porosity (24.67 nm avg. pore diameter, 5.583 m 2 /g surface area) facilitated rapid diffusion kinetics (equilibrium within 16 h). DFT calculations correlated dye selectivity with electronic properties, identifying MV's low energy gap (ΔE GAP = 2.686 eV) and high dipole moment (μ = 2.004 D) as key drivers for enhanced π-π and electrostatic binding. Adsorption followed pseudo-second-order kinetics (R 2 > 0.993) and Sips isotherm models (R 2 > 0.997), confirming chemisorption-driven multilayer mechanisms. Despite robust regeneration (>78 % efficiency over five cycles via 0.10 M HCl), gradual capacity decline highlighted challenges in Ca 2+ -H + exchange stability. The aerogel's dual-function design, combining tunable surface chemistry with structural resilience, positions it as a scalable, high-performance solution for sustainable wastewater remediation.
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ChemSusChem
·
2025
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IF 6.6
Zixuan Tan,Yihong Cai,Bo Yang,Hao Huang,Haijun Guo,Min Zhuang,Hui Luo,Qingwei Meng,Shaoqu Xie
Graphical Monohydric alcohols are a potential fuel, and herein, monohydric alcohols have been selectively synthesized from multicarbon sugars by modulating the electron distribution of Ru and enhancing the hydrodeoxygenation process of biomass. Ru-based catalysts are widely used in catalytic reactions, but the electron-deficient nature promotes strong decarbonylation, leading to complete deoxygenation during the conversion of polyhydroxy biomass. Despite extensive research, effectively suppressing this decarbonylation activity remains challenging. Herein, electron-rich Ru and electron-deficient Ni formed due to the electron migration of Ni → Ru have a synergistic catalytic effect, controlling the precise cleavage of C N bonds by Ru 0 and retaining most of the C O bonds. The amorphous Al 2 O 3 is sufficiently bound to the substrate to promote rapid hydrogenation. This modification effectively suppresses the intrinsic decarbonylation activity of Ru and improves selectivity for hydrodeoxygenation. Using carbohydrates as substrates, the Ru–Ni bimetallic catalysts preferentially promote the hydrodeoxygenation pathway, resulting in a significant increase in C3+ monohydric alcohol yields. This work presents a new strategy for modulating reaction pathways via electronic structure engineering, offering valuable insights into the potential of Ru–Ni systems for biomass conversion and sustainable alcohol synthesis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
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IF 6.3
Zhengyan Hao,Zhiwei Zhang,Xijia Yang,Xuesong Li,Yang Gao,Liying Wang,Yuxin Huang,Wei Lü
Zinc-ion hybrid supercapacitors (ZIHSCs) have garnered widespread attention due to their integration of the excellent characteristics of both batteries and capacitors. This study employs a synergistic strategy combining hydrothermal and high-temperature calcination methods to construct a nanosphere-structured T-Nb 2 O 5 composite anode material coated with reduced graphene oxide (rGO) on a flexible carbon cloth (CC) substrate (T-Nb 2 O 5 /rGO@CC), in conjunction with a hierarchical super-mesoporous activated carbon cathode (ACcp@CC) derived from discarded citrus peel. The rGO coating structure suppresses the volume expansion of the internal nanostructure caused by charging and discharging, effectively enhancing mechanical stability. At the same time, the three-dimensional conductive network of rGO effectively compensates for the poor intrinsic conductivity of Nb 2 O 5 . The constructed ZIHSC delivers a capacitance of 718.56 mF cm −2 at 1 mA cm −2 , and achieves a maximum energy density of 399.20 μWh cm −2 at 1 mW cm −2 . Furthermore, after 50,000 ultralong-cycle, the capacity retention rate is 104.17 %. The assembled flexible device not only possesses excellent mechanical properties but also delivers a specific capacitance of 389.89 mF cm −2 at 1 mA cm −2 , providing long-term power for various electronic devices. This study provides a solid theoretical reference for the design of stable composite structures and the investigation of ultra-long cycling performance in niobium-based electrode materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Changsheng Wu,Zhiyong Wang,Xianbo Jin
Niobium (Nb) is primarily used as the active material in Nb electrolytic capacitors in the form of metallic fine powder. Unlike traditional methods of preparing niobium powder through chemical or electrochemical reduction of metal compounds in molten salts, we report here the efficient preparation of Nb nanopowder via electrolysis of NbS 2 in the NaCl-KCl melt at 973 K. The NbS 2 is simply synthesized by carbo-sulfidation of Nb 2 O 5 . The following electro-desulfidation in the molten electrolyte converts solid NbS 2 into Nb nanopowder at the cathode, with S 2- ions moving to the anode and being oxidized to gaseous sulfur. The reduction path was verified to be NbS 2 → L x NbS 2 → NbS 2-w → Nb. Through constant cell electrolysis at 2.9 V, NbS 2 is rapidly reduced to nodular Nb nanopowder (50-100 nm), with a Current efficiency and energy consumption of approximately 94% and 3.58 kW·h kg⁻¹ Nb, respectively.
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Advanced Sustainable Systems
·
2025
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IF 6.1
Zhongyang Qian,Jiaojing Hu,Jingbo Chao,Jinlou Huang,Frederic Coulon,Jingqi Zhang,Qing Hu,Xiao Jin Yang
The efficient and sustainable in situ remediation of high-strength acidic groundwater contaminated by complex micropollutants with minimal use of chemicals is a challenge. Here it is reported that MgAl alloy achieves neutralization and a complete removal of 20 mg L −1 Cd 2+ , Cr(VI), Cu 2+ , Ni 2+ , and Zn 2+ in 15 min from acidic water free of chemicals. The removal rate of heavy metals and nitrate increases with decreasing pH and is not significantly reduced after 5 cycles of treating acidic water. The excellent performance of MgAl alloy in reactivity, durability, and efficiency is attributed to a synergistic effect of chemical reduction and eutectic reactions, which is catalyzed by intermetallic compound Mg 17 Al 12 and in situ layered double hydroxide (iLDH). The pH 2.47 of an acid mine drainage sample from copper ore mines is raised to 7.4 ± 0.4 and the concentrations of Al, Cr, Cu, Fe, Mn, Ni, and Zn ions are reduced to <0.55 mg L −1 from 5–559 mg L −1 . In contrast, quick lime treatment increases the pH to 12.45, whereas activated carbon, zerovalent iron, and conventional LDH are not able to neutralize or remove Al 3+ and heavy metals. The findings of this study provide new insights into the efficient, green, and sustainable approach for acidic water remediation.
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Science China-Chemistry
·
2025
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IF 9.7
Yang Yaqiong,Lv Tian-Run,Xue Yi-Han,Yin Zhigang,Yin Ming-Jie,An Quan-Fu
Real-time monitoring of ion content variations in humans offers a noninvasive approach to ensuring health, made possible through wearable sensors. However, challenges such as the low capacitance of the solid-contact (SC) layer and the formation of a water layer hinder the low-concentration ion detection and stable performance of these sensors. To address these limitations, a novel design is proposed using graphene quantum dots (GQD)-doped polypyrrole (PPy) nano-dendritic membranes, combined with a hydrophobic Nafion membrane, for sweat ion sensors. The GQD-doped PPy membrane serves as the SC layer, where GQD enhance capacitance and the nano-dendritic structure improves ion-to-electron transduction efficiency. Meanwhile, the hydrophobic Nafion membrane prevents water layer formation, stabilizing the sensor’s performance. This design significantly improves both the sensitivity (from 49 mV/decade to 70 mV/decade) and stability (potential drift decreasing from 1.3 mV/h to 18.7 μV/h) of the sensor. Leveraging this configuration, Na + and K + sensors are integrated onto a flexible electrode using a dispense-coupled inkjet printing technique. This enables real-time, continuous monitoring of Na + and K + concentrations in human sweat simultaneously. The proposed sensing device demonstrates strong potential for noninvasive sweat monitoring, contributing to enhanced health management in daily life.
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