ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 34
·46312-46321
·
IF 7.8
Wang Guangxia,Sun Xiuwei,Geng Ruyang,Xu Yong,Hu Tao,Qiu Zhenping
The commercialization of direct alcohol fuel cells (DAFCs) is severely hindered by sluggish anodic alcohol oxidation reaction kinetics and the high susceptibility of catalysts to deactivation. Traditional Pd/Pt-based catalysts suffer from difficult C−C bond cleavage and severe CO poisoning. To address these issues, we synthesize a pentametallic PdPtNiBiCo alloy consisting of interconnected nanoparticles via a facile one-pot oil-phase method, aiming to maximize electrochemically accessible surface sites and trigger robust multimetallic synergy. This architecture delivers an exceptional alkaline ethanol oxidation activity of 16.64 A mg −1 Pd+Pt , 12 and 19 times higher than those of commercial Pd/C and Pt/C, respectively. Furthermore, the catalyst exhibits robust antipoisoning durability over 4000 cycles and broad activity for methanol and ethylene glycol oxidation. Density functional theory calculations reveal that multimetallic synergy effectively modulates the d-band center of the active sites. Density functional theory calculations reveal that multimetallic synergy tunes the electronic structure of the active sites, optimizes the adsorption of key intermediates, and lowers the thermodynamic energy requirements for C−C bond cleavage and CO oxidation, thereby facilitating both the C1 and C2 pathways of ethanol oxidation. This work addresses the key limitation of traditional Pd/Pt-based catalysts and provides an effective strategy for designing high-performance universal DAFC anodes.
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CRYSTAL GROWTH & DESIGN
·
2026
·Vol. 26
·期 17
·7189-7200
·
IF 3.6
Chen Yuliang,Wang Qibo,Xu Qinqin,Wu Wenhua,Zhao Liwei,Cheng Tong,Yin Jianzhong
Three-dimensional MoS 2 structures provide
enriched interlayer
coupling, abundant edge/step sites, and thickness gradients, opening
opportunities for tailoring electronic and interfacial functionalities.
Controlled growth of pyramidal MoS 2 remains challenging
because its structure is governed by precursor supply, local supersaturation,
and secondary nucleation. Herein, we report a droplet-mediated vapor–liquid–solid
CVD strategy for the controllable growth of pyramidal MoS 2 using precursor-rich Na–Mo–O droplets as localized
precursor reservoirs and reaction interfaces. Statistical analysis
reveals a correlation between droplet diameter and pyramid lateral
size, indicating the strong coupling between droplet-mediated supply
and crystal growth. Combined classical nucleation theory and DFT calculations
support a supersaturation-governed growth transition. Under low effective
interfacial supersaturation, upper-step nucleation is less accessible
and lateral growth is favored, whereas increasing effective interfacial
supersaturation progressively facilitates secondary nucleation and
step stacking. KPFM further reveals a stepwise evolution of surface
potential along the thickness gradient. Despite the microscale channel
thickness and interlayer screening, back-gated transistors based on
pyramidal MoS 2 remain electrically addressable, exhibiting
apparent two-terminal field-effect mobilities of 4–6 cm 2 V –1 s –1 and on/off ratios
on the order of 10 3 . This work establishes a controllable
route to thickness-graded three-dimensional MoS 2 structures
and provides mechanistic insight into stacking growth in layered semiconductors.
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ACS Catalysis
·
2026
·Vol. 16
·期 17
·17113-17124
·
IF 13.6
Wang Jiahao,Teng Rui,Sun Yunshuyu,Zhang Meng,Mao Yuxiang,Ma Ruixue,Wang Kangbo,Lv Hongkun,Zhang Kang,Chen Jiayin,Xia Rongxin,Cheng Jun
Molecularly dispersed cobalt phthalocyanine (CoPc) on carbon nanotubes can be used as an efficient catalyst for electrochemical CO 2 -to-methanol conversion. However, increasing the CoPc loading to enhance the current density typically induces aggregation, which compromises methanol selectivity. To overcome this limitation, a CNT-supported nitro-substituted CoPc electrocatalyst (nCoPc@CNT) that adopts a distinct molecular-cone configuration was developed in this work, differing from both molecularly dispersed and aggregated structures. Structural analyses confirm that this molecular-cone configuration increases the density of electrochemically accessible sites while maintaining favorable catalytic activity. Combined theoretical and experimental analyses suggest that the molecular-cone architecture establishes an optimized interfacial microenvironment, in which the electric-field enhancement predicted by COMSOL is associated with local K + enrichment and stabilization of the key *CO intermediate. Concurrently, interfacial water structures are reorganized to form a strengthened hydrogen bond network that promotes proton transport and accelerates *CO hydrogenation kinetics, as evidenced by a shortened DRT low-frequency relaxation time. Leveraging this microenvironment, the molecular-cone nCoPc@CNT catalyst achieves a methanol Faradaic efficiency of 64.4% at –0.98 V vs RHE and retains a Faradaic efficiency of 58.4% at 150 mA cm –2 in a membrane electrode assembly (MEA) cell. This work presents a microenvironment-engineering strategy for selective electrochemical CO 2 reduction to methanol via cooperative interfacial tuning.
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ACS Catalysis
·
2026
·Vol. 16
·期 16
·16055-16065
·
IF 13.6
Wang Yanlin,Gu Panpan,He Ruoyan,Xue Qizhou,Cheng Aofei,Liu Xiang,Zeng Shaojuan,Wang Min,Zhang Zhenlei,Zhang Kaihang,Feng Jiaqi,Zhang Xiangping
The electrochemical CO 2 reduction reaction (CO 2 RR) is a proton−electron coupled transfer process in which active hydrogen (*H) plays a pivotal role in determining the reaction pathways, particularly for methane (CH 4 ), a representative deep hydrogenation product. However, how *H generation and migration govern CH 4 formation remains elusive, motivating mechanistic elucidation to enable rational regulation of reverse hydrogen spillover. Herein, we develop Cu-doped ZrO 2 catalysts and reveal that tuning the crystallinity of the ZrO 2 support enables control over the reverse hydrogen spillover process. Specifically, amorphous ZrO 2 functions as an efficient “hydrogen pump” by promoting *H generation and lowering the migration barrier toward adjacent Cu sites, thereby strengthening the reverse hydrogen spillover effect. This effect establishes an optimal *H coverage for deep hydrogenation of CO 2 , thereby reducing the energy barriers for key intermediates along the CH 4 formation pathway. Consequently, the Cu-doped amorphous ZrO 2 catalyst delivers a CH 4 Faradaic efficiency of 69.3% with a partial current density of −372.8 mA cm −2 , significantly surpassing that of its crystalline analogue. This work highlights that engineering the crystallinity of metal oxide supports provides an effective strategy to regulate reverse hydrogen spillover in electrocatalysis, offering valuable insights into controlling catalytic activity and product selectivity.
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 35
·20723-20730
·
IF 4.6
Cong Shenzhen,Sun Si,Wang Ming,Zhang Yijing,Shen Qin,Zhang Yatao,Pang Huan
Membrane-based separation technology holds great promise
for CO 2 capture, yet conventional membranes are often constrained
by the permeability-selectivity trade-off. In this study, we developed
a zirconium-cluster (Zr 6 )-incorporated ZIF-8 membrane via
an electrochemical synthesis strategy to address this limitation.
The resulting Zr 6 @ZIF-8 composite membrane exhibits high
crystallinity, a dense microstructure, and homogeneous dispersion
of Zr 6 clusters within the ZIF-8 framework. The optimized
Zr 6 @ZIF-8–2 membrane demonstrates outstanding CO 2 separation performance with a CO 2 permeance of
up to 300.0 gas permeation unit and CO 2 /N 2 and
CO 2 /CH 4 selectivities of 27.0 and 14.8, respectively.
The Zr 6 clusters enable effective structural regulation
of ZIF-8 membranes, resulting in enhanced CO 2 separation
performance and leading to improved diffusion selectivity. Furthermore,
the membrane shows a stable separation performance under varying feed
pressures and temperatures, along with excellent long-term operational
stability. This work provides an effective electrochemical approach
for fabricating high-performance MOF-based membranes, offering a promising
candidate for industrial CO 2 capture and natural-gas purification.
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ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 35
·15995-16008
·
IF 7.6
Zhang Wenlin,Liang Siqi,Ma Chuanguo,Liu Yuqi
Multifunctional benzoxazine resins with high‑rigidity skeletons have gained widespread research interest owing to their comprehensive performance advantages, but their monomers typically suffer from high melting points and poor solubility. To address this issue, three multifunctional benzoxazines, DATR-fa, DAHT-fa, and DPAHT-fa, were synthesized in the green solvent ethanol using biomass-derived phenolic acids, phenolic alcohols, and furfurylamines. All three monomers exhibit low melting points (81, 93, and 61 ° C), which are attributed to the introduction of ester groups and short alkyl chains that weaken molecular rigidity and packing regularity. Through thermal curing, three cured resins, poly(DATR-fa), poly(DAHT-fa), and poly(DPAHT-fa), were prepared, all of which exhibit excellent heat resistance (glass transition temperatures of 266, 286, and 296 ° C), high thermal stability (initial decomposition temperatures of 353, 341, and 359 ° C), and good flame-retardant properties (heat release capacity (HRC) values of 65.4, 46.4, and 61.8 J/(g·K), total heat release (THR) values of 6.4, 4.7, and 5.0 kJ/g, and UL-94 ratings of V1, V0, and V1, respectively). Furthermore, a detailed study was conducted on the flame-retardant mechanism of these polybenzoxazine resins. This work offers new guidelines for designing multifunctional benzoxazine resins featuring balanced processability, thermal stability, and intrinsic flame retardancy.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 35
·47618-47628
·
IF 7.8
Zhang Zhao,Li Renjie,Ding Zhao,Wang Sa,Du Aoxuan,Wang Dan,Xie Wei
The development of efficient and reversible ammonia (NH 3 ) adsorbents is crucial for advancing ammonia fuel cell technology. Key challenges in the ammonia adsorption–desorption process include achieving high uptake/release efficiency, favorable kinetics, and stable cycling lifetime. Herein, we report a strategy to prepare high-performance ammonia adsorbents by partially etching metal–organic frameworks (MOFs) with tannic acid (TA). Partial etching by protonated TA not only exposes metal active sites but also chelates metal ions, significantly enhancing both the adsorption capacity and the stability during adsorption–desorption cycles. This strategy retains the high specific surface area of the micropores and the chelating functional groups while alleviating premature pore blockage caused by capillary condensation of ammonia on the material surface, thereby improving adsorption kinetics. The partially etched ZIF-67 achieves a reversible capacity as high as 58 mmol g –1 at 298 K and 7 bar, theoretically corresponding to a hydrogen content of 7.5%. The generated hierarchical pore network facilitates ammonia desorption, reducing the temperature and energy required for regeneration, with complete desorption achieved at 364 K. Moreover, the partially etched MOF exhibits excellent ammonia adsorption selectivity, offering a new approach for the purification of industrial exhaust gases. In situ infrared spectroscopy and theoretical calculations reveal that the enhanced adsorption arises from weak chemisorption, benefiting from an increased density of adsorption sites within the engineered pore environment. This strategy provides a new avenue for designing integrated, efficient, and safe systems for ammonia fuel storage and release.
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Surfaces and Interfaces
·
2026
·
IF 6
Jiahui Fan,Fengxiang Liang,Qingshuo Liu,Zongyuan Cao,Zhuo Zhang,Bin Chen,Peng Zhang
S-CeNiFe LDH/NiS 2 enhances the durability of seawater splitting. • Sacrificial NiS 2 nanoparticles protect catalyst from Cl- corrosion. • Sulphuration and Ce atoms mitigate the loss of Ni/Fe during seawater splitting. • Downshifted d-band optimizes the OER and suppresses ClER. The development of efficient and stable electrocatalysts to overcome chloride corrosion is crucial for sustainable hydrogen production via alkaline seawater electrolysis. Herein, a Ce-doped NiFe LDH heterostructure (S-CeNiFe LDH/NiS 2 ) was synthesized and exhibited enhanced bifunctional activity for both the oxygen and hydrogen evolution reactions (OER/HER) in alkaline seawater (1 M KOH + natural seawater), along with seawater corrosion resistance by the sacrificial NiS 2 nanoparticles. The optimized S-Ce 0.4 NiFe LDH/NiS 2 requires low overpotentials of only 310 mV for OER and 290 mV for HER at 100 mA cm -2 , surpassing both unsulfurated CeNiFe LDH and bare NiFe LDH. It also shows smaller Tafel slopes and maintains excellent stability over 100 h with minimal decay. The sacrificial role of NiS 2 in protecting LDHs is confirmed by its structural and chemical evolution alongside attenuated seawater decomposition. Performance enhancement stems from heterostructure synergy: expanded surface area, accelerated charge transfer, Ce doping-induced electronic modulation, and conductive NiS 2 for HER. This work addresses critical challenges in direct seawater splitting for scalable hydrogen production. Download: Download high-res image (264KB) Download: Download full-size image
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2026
·
IF 8.7
Xingyue Liu,Wen Deng,Liucheng Meng,Jianfeng Xi,Chaofeng Zhang,Jinlan Cheng,Lei Zhang,Huining Xiao,Weibing Wu
Conventional synthetic routes to Ag nanocubes (AgNCs) often leave reagent residues on the particle surface, thereby compromising analyte accessibility and surface-enhanced Raman scattering (SERS) sensitivity. Here, AgNCs were grown in-situ on two-dimensional (2D) nanocellulose films via a photo-induced reduction process, yielding surfactant-free particles with tunable morphology. No additional reducing agents or surfactants were introduced during synthesis, reducing surfactant-derived surface coverage and improving the accessibility of the resulting AgNCs. Notably, the dissolved oxygen in the reaction solution played an important etching role in eliminating the twins during the nucleation process and generating AgNCs with a single crystal structure. The nanocellulose film served both as a photo-reactive substrate, where surface hydroxyl groups acted as reductive sites for the photo-induced conversion of Ag(I) to Ag(0), and as a 2D support that stabilized interfacial nucleation and growth. In addition, the in-situ synthesized AgNCs were uniformly distributed across the nanocellulose film surface, enabling one-step fabrication of flexible SERS substrates under mild conditions. The optimized substrate enabled highly sensitive detection of Rhodamine 6G (R6G), with a limit of detection of 6.24 × 10 −12 g L −1 , approximately fivefold lower than that of the same substrate after surfactant adsorption. This strategy provides a simple platform for constructing nanocellulose-based SERS substrates for trace detection.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Chunyan Zhang,Wenke Xie,Wenliang Li,Na Li,Lingxiang Zhang,Yuxiang Zhong,Liang Sun,Wenjun Li,Songtao Cai,Hu Chen,Zhongchang Wang,Jianxin Luo
Highly defective UiO-66 was prepared using a one-pot solvothermal approach with benzoic acid as a defect modulator. • The pore structure and hydrophilicity of UiO-66 can be regulated by tuning the load of benzoic acid. • BPA adsorption by UiO-66-B3 is a spontaneous exothermic process dominated by monolayer chemisorption. • The excellent BPA adsorption performance of UiO-66-B3 arises from a synergistic process. UiO-66, a Zr-based metal-organic framework (MOF), shows great potential in adsorption, catalysis, water treatment, and chemical shielding. Defect engineering has been employed to further enhance its adsorption performance. Nevertheless, conventional defective UiO-66 suffers from time-consuming synthesis and fragile porous structure, and its adsorption capacity needs further improvement. In this study, a highly defective UiO-66 (denoted as UiO-66-BX, where X = 0, 1, 2, 3, 4, and 5) was synthesized using a one-pot solvothermal approach, with BA as the defect modulator to trigger competitive coordination. Its adsorption performance was demonstrated using bisphenol A (BPA). The results demonstrated that the adsorption data of the UiO-66-B3 for BPA in wastewater were well-fitted by the pseudo-second-order kinetic model and the Langmuir model, and both Δ G and Δ H were below 0, indicating that it is a spontaneous exothermic process dominated by monolayer chemisorption. Meanwhile, the theoretical adsorption capacity of the UiO-66-B3 can be up to 340.14 mg∙g −1 at 298.15 K. Additionally, adsorption by the UiO-66-B3 showed excellent tolerance to high ionic strength (variation in the adsorption capacity <7%) and good reusability (variation in adsorption capacity <10%). The excellent adsorption performance of the UiO-66-B3 can be attributed to a synergistic process involving mesopore-induced pore filling, hydrogen bonding between Zr-OH sites and phenolic -OH, coordination bonding between Zr 4+ and O in -OH, and π-π stacking of benzene rings. This study provides a promising strategy for the development of defect-rich UiO-66 for efficient pollutant removal. Download: Download high-res image (210KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Haiyang Yu,Xiaojing Sun,Xinyue Song,Chuan Liang,Tongtong Zhou,Tao Wang
Sp 3 -type edge defects and sp 2 -type pentagonal defects were precisely engineered. • EDC prefers electron-donating ECs, while PDC favors electron-accepting ones. • π-π EDA interactions dominate the selective adsorption of ECs. • Defect configuration governs electronic matching for selective ECs removal. The persistent release of emerging contaminants (ECs) into water systems poses significant risks to human health and ecosystems. Adsorption using carbon-based materials offers a sustainable remediation strategy, yet the role of intrinsic defects in preferential contaminant removal remains poorly understood. Herein, we engineered two carbon-based materials with distinct defect configurations: one enriched with sp 3 -type edge defects (EDC) and another with sp 2 -type pentagonal ring defects (PDC), as unequivocally corroborated by aberration-corrected scanning transmission electron microscopy (ac-STEM) and complementary characterizations. Batch adsorption experiments were conducted using six ECs of opposite electronic nature, including antibiotics, DNA bases, and nanoscale plastics. Remarkably, PDC exhibited superior adsorption capacities for electron-accepting contaminants with values of 392.5 mg g −1 for norfloxacin, 249.1 mg g −1 for cytosine, and 115.3 mg g −1 for PS-COOH, while EDC showed superior adsorption capacities for electron-donating ones with values of 469.5 mg g −1 for amoxicillin, 230.5 mg g −1 for adenine, and 129.5 mg g −1 for PS-OH. Mechanistic studies, combining preferential desorption and density functional theory calculations, revealed that π-π electron donor-acceptor interactions, governed by the distinct HOMO/LUMO energies of the defects, dominate the adsorption process. Biomass-derived counterparts exhibited consistent preferential adsorption, confirming that the defect-engineering approach yields similar trends across the tested precursors. This suggests a potentially extendable strategy and offers an electronic-matching paradigm for the preferential removal of diverse ECs based on their intrinsic electronic properties. Download: Download high-res image (380KB) Download: Download full-size image
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TALANTA
·
2026
·
IF 6.7
Wei Zhang,Jinhui Wang,Jialu Xu,Yulong Xu,Haiyan Li,Yujun Jiang
The environmental persistence and inherent biodegradation resistance of pesticide residues pose a serious threat to ecosystems and human health, necessitating the development of efficient monitoring strategies. Herein, we decipher the fluorine-fluorine (F···F) interaction within an AIE-active, trifluoromethyl-functionalized covalent organic framework (PEFA-COF) and exploit this molecular recognition motif for the selective detection of trifluralin (TFR). Benefiting from abundant trifluoromethyl moieties and superior luminescence properties, the PEFA-COF enables specific TFR recognition through a synergistic interplay of electrostatic forces, hydrogen bonding, and F···F interactions. This recognition event triggers a pronounced fluorescence quenching response via the internal filtration effect (IFE), facilitating highly sensitive and selective TFR quantification. The constructed PEFA-COF-based fluorescent sensing platform was successfully validated in complex water and milk matrices, achieving an excellent fluorescence quenching coefficient and a detection limit as low as 0.06 μmol/L. Collectively, this work not only deciphers the critical role of F···F interaction in pesticide recognition but also advances the function-led design of AIE-active COFs toward practical and robust pesticide residue monitoring in food supply chains.
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危险品化学品经营许可证（带存储）