APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Qiankun Xu,Rui Wang
MOF-derived NiCo/NPC electrocatalyst was constructed with tailored M-N 4 coordination environments. • Ni incorporation regulated Co electronic structures for accelerated oxygen evolution reaction. • DFT calculations elucidated the electronic modulation mechanism and optimized OER energetics. The development of efficient, low-cost, and scalable oxygen evolution reaction (OER) catalysts is crucial for practical water electrolysis. Herein, a MOF-derived NiCo/NPC electrocatalyst containing predominantly atomically dispersed Co–N 4 /Ni–N 4 sites is prepared by controlled Ni incorporation into ZIF-67-derived porous carbon. The optimized 50% NiCo/NPC exhibits an overpotential of 207 mV at 10 m⋅A cm⁻ 2 , a Tafel slope of 51.6 mV⋅dec⁻ 1 , and stable operation for over 100 h, outperforming Co/NPC and commercial RuO 2 . Aberration-corrected HAADF-STEM directly visualizes atomically dispersed Co and Ni species, while synchrotron X-ray absorption spectroscopy confirms the Co–N 4 coordination environment and reveals that Ni incorporation modifies the electronic environment of the Co sites. Density functional theory calculations further show that Ni incorporation shifts the Co d -band center toward the Fermi level and lowers the energy barrier of the rate-determining step, accounting for the enhanced OER activity. In an anion exchange membrane water electrolyzer, the catalyst delivers current densities of 1000 and 4000 mA ⋅cm⁻ 2 at 2.02 and 2.46 V, respectively. This work provides an effective strategy for improving the OER performance of MOF-derived electrocatalysts through regulating the electronic structure of Co active sites. Download: Download high-res image (186KB) Download: Download full-size image Ni-doped ZIF-67 is converted via pyrolysis into morphology-retained Co–N 4 and Ni–N 4 single-atom active sites embedded in N-doped porous carbon (NiCo/NPC). Benefiting from the Ni-induced electronic modulation of Co active sites, together with the enhanced conductivity of the carbon framework, the catalyst achieves efficient and durable OER performance with a low overpotential.
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Nature Communications
·
2026
·
IF 18.1
Tian Kaige,Wang Xianhui,Xiang Pengyu,Zhao Jingyi,Li Yan,Liu Chenghang,Wang Chengbo,Liu Xiao,Fu Donglong,Ma Xinbin,Pei Chunlei,Chen Sai,Gong Jinlong
Strongly endothermic reactions are always constrained by thermodynamic equilibrium that necessitates high-temperature operation. This paper describes a co-thermal coupling strategy that integrates two thermodynamic equilibrium-limited processes into a single reaction environment via hydrogen transfer. In this system, the hydrogen generated in situ from endothermic propane dehydrogenation is continuously consumed by simultaneous carbonate decomposition, thereby achieving bidirectional reaction intensification. As a result, the decomposition temperature of calcium carbonate is reduced by approximately 75 °C compared to inert conditions, while the propane dehydrogenation conversion reaches ~120% of the thermodynamic equilibrium value with a propylene selectivity of 97.8% during the continuous regeneration cycles. In situ spectroscopic and kinetic analyses demonstrate a coupled reaction network, where hydrogen transfer promotes carbonate transformation via bicarbonate-related surface intermediates and then follows the reverse water-gas shift pathway. Techno-environmental analysis indicates that this integrated process lowers the energy consumption per ton of propylene by 9.8% and reduces net CO 2 emissions by 18.1% in the base-case industrial simulation, while co-producing propylene and a CaO-containing solid. These findings establish hydrogen-mediated co-thermal coupling as a general strategy for surmounting equilibrium constraints and intensifying energy- and carbon-intensive chemical processes.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
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IF 3.5
Xiaofu Li,Tingfeng Xue,Junliang Ma,Zhibo Liu,Zejia Song,Bingyan Zhu,Liwei Pan,Jing Zhang
A bimetallic Mn-Co@γ-Al 2 O 3 catalyst was prepared • The catalyst effectively activates PMS for the mineralization of CIP • The catalyst enhances PMS activation via electronic, structural and active-site synergy • 1 O 2 is synergistically generated by LAS, oxygen vacancies and bimetallic redox cycles Ciprofloxacin (CIP) is recalcitrant to complete degradation by conventional treatment methods, and persulfate-based advanced oxidation processes often suffer low activation efficiency. In this study, a bimetallic Mn-Co@γ-Al 2 O 3 catalyst was developed to activate peroxymonosulfate (PMS) for the efficient mineralization of CIP. Under optimal conditions (1 mmol·L -1 PMS, pH=9), CIP was completely mineralized within 60 min. The catalytic activity of the bimetallic catalyst surpassed that of the single-metal Mn@γ-Al 2 O 3 and Co@γ-Al 2 O 3 , with a synergistic factor ( SF =1.12, >1) confirming a strong Mn-Co synergy. This synergistic effect results from coupled redox cycles, the inhibition of manganese oxide aggregation, and the presence of abundant Lewis acid sites and oxygen vacancies. The PMS system, primarily governed by singlet oxygen ( 1 O 2 ), effectively reduced the biotoxicity of CIP wastewater, increasing the germination rate of fescue seeds from 80% to 92%. A total of 14 degradation intermediates were identified. The excellent mineralization performance is closely associated with the unique CIP degradation pathway driven by 1 O 2 .
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Nature Communications
·
2026
·
IF 18.1
Wang Xiao-hong,Liu Xu-jia,Wang Yun-biao,Li Yi-lei,Liu Shao-jia,Mu Hui-ying,Li Fa-tang
Revealing the mechanism of photocatalytic organic transformation in aqueous solutions is crucial for photocatalytic processes, yet precisely regulating complex interfacial electron transfer and the microenvironment of reaction molecules remains challenging. Inspired by cellular structures and natural metalloproteins, we construct a ZIF-67@CoS/CdS nanoreactor mimicking organelle architecture. This system enables directional charge transport and hydrogen-bond microenvironment regulation, allowing efficient co-production of H 2 and pyruvic acid under light irradiation. Characterizations and calculations reveal that the interfacial electric field accelerates charge migration, while the catalyst reduces the energy barriers for water dissociation and hydrogen formation by modulating hydrogen bonds. The optimized catalyst delivers a molar-level H 2 activity of 1457.1 mmol m −2 (5 h, 1,000 cm 2 ) under sunlight, with a pyruvic acid selectivity of 91.2%. In this work, we propose a design strategy for an organelle-mimetic nanoreactor for scalable sunlight-driven H 2 production and selective pyruvic acid synthesis.
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Polymers
·
2025
·Vol. 17
·期 12
·1702
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IF 4.9
Ningxin Ma,Wenzheng Xu,Xiaolong Chang,Shuying Lan
The issue of interfacial inhomogeneity in energetic materials remains a significant challenge. In this study, fluoroelastomer F2602 was applied to HMX crystals using a water suspension granulation technique, followed by a bio-inspired coating formed via the crosslinking polymerization of polyethyleneimine (PEI) and pyrogallol (PG) on the HMX/F2602 composite. This process resulted in the formation of an HMX/F2602/PEI-PG microcapsule structure. Various characterization techniques confirmed that the chemical structure and polycrystalline morphology of the crystals were preserved throughout the coating process, maintaining the characteristic β-HMX morphology. The introduction of the PG–PEI shell significantly improved the coating coverage and minimized the exposure of crystal surfaces. Furthermore, compared to HMX/F2602, the HMX/F2602/PEI-PG composite exhibited notably enhanced thermal stability and reduced mechanical sensitivity. These improvements are attributed to the advantageous effects of the microcapsule structure formed by the bio-inspired coating on the material’s properties.
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Materials Horizons
·
2025
·
IF 10.7
Ziqing Yuan,Jiasu Xu,luyao li,Hongxia Li,Jie He,Kaiwen Bao,Lai Jiang,Guangxia Shen,Xianting Ding
Visualization of proteins and nucleic acids with super-resolution is a persistent need. Expansion microscopy (ExM) permits nanoscale imaging of biomolecules on conventional microscope by physically expanding biological specimens embedded in a stretchable hydrogel. However, achieving simultaneous super-resolution co-imaging of proteins and nucleic acids on ExM has remained a general challenge. Here, we present photoclick dual anchoring expansion microscopy (Phan-ExM), which employs an unorthodox anchoring reagent, N-(3-methacrylamidopropyl)-3-(2-methyl-1 H-pyrrol-1-yl)-2 H-tetrazole-2-carboxamide (MAP-mPyTC), for rapid and concurrent retention of proteins and nucleic acids within the ExM gel matrix through photoclick chemistry. We demonstrated MAP-mPyTC could anchor both protein and mRNA biomolecules within 10 minutes, significantly reducing the time compared to typical ExM techniques, which usually take several hours to overnight. Moreover, we showed that Phan-ExM significantly enhanced the fluorescence intensity of protein and RNA spots compared to previous method. With Phan-ExM, we achieved high-resolution co-imaging of multiplex proteins and nucleic acids on a single specimen at ~85 nm resolution. We revealed that paclitaxel and colchicine treatment significantly disrupted mitochondrial dynamics in BALB/c 3T3 cells, with an associated aggregation of ACTB mRNA observed at sites of mitochondrial damage. Phan-ExM provides a platform technique for super-resolution colocalization of nucleic acids and proteins on the same specimen with conventional microscope.
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ACS Nano
·
2025
·
IF 16
Yong Liu,Honglei Wang,Yun Song,Charles B. Musgrave III,Pei Xiong,Jiangtong Li,Geng Li,Libei Huang,Jianjun Su,Yinger Xin,Qiang Zhang,Weihua Guo,Mingming He,Tanglue Feng,Xing Li,Molly Meng-Jung Li,Peter A. van Aken,Hongguang Wang,William A. Goddard III,Ruquan Ye
Spatially arranged molecular catalysts in polymeric frameworks, typically in a layered structure, are emerging strategies to mitigate the molecular aggregation and improve the catalytic performance. However, the effect of local coordination induced by polymerization remains underexplored. Here, we develop one-dimensional cobalt-tetra-amino-phthalocyanine-based covalent organic polymers (1D-COP) for the electrochemical CO reduction reaction (CORR). We use carbon nanotubes as ideal templates to induce local curvature of the 1D-COP. The COP on single-walled CNT (1D-COP/SWCNT) catalyst exhibits a maximum methanol Faradaic efficiency of 70% in an H-cell, which exceeds those on wider-diameter multiwalled carbon nanotubes (22% for 4–6 nm and 14% for 10–20 nm). Using X-ray and vibronic spectroscopies, we have observed distinct local geometries and electronic structures induced by the strong interactions between the COP layer and CNT substrates. Density functional theory calculations further support that increased curvature of the COP-SWCNT catalyst enhances the *CO binding species, leading to improved subsequent reduction reactions. Our results highlight the critical role of the local structure in polymeric frameworks for improved electrocatalytic performance.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 11
·1-15
·
IF 2.4
Yang Dawei,Hu Yanan,Qi Zhiwei,Li Qiaoling,Yu Chengcheng
The world is currently facing the dual challenges of energy scarcity and environmental degradation. As a highly promising carrier of clean and renewable energy, hydrogen has attracted significant attention, with high-efficiency water electrolysis recognized as a key pathway for the large-scale production of green hydrogen. Among various electrocatalysts, transition metal Co-V-based materials demonstrate remarkable potential. In this study, we successfully synthesized a highly stable amorphous Co-V-B catalyst on a nickel foam (NF) substrate by constructing a Co-V bimetallic system followed by boron doping to enhance its performance. Electrochemical evaluations indicated that the catalyst delivers superior Hydrogen evolution reaction (HER) performance, requiring only 47 mV overpotential to attain a current density of − 10 mA cm −2 , along with a low charge transfer resistance of 1.14 Ω. Additionally, the catalyst demonstrated remarkable durability, sustaining stable HER activity during 16 h of continuous chronopotentiometric (CP) operation. This study systematically explores the preparation of Co-V/NF catalysts and highlights the significant impact of boron incorporation on improving catalytic performance, providing meaningful guidance for developing advanced electrocatalysts for water splitting applications. Graphical
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JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Linfeng Zhang,Yan Cao,Jie Li,Chao Li,Yanlin Yang,Jiao Li,Xuewei Hu,Xiangfen Cui,Qun Zhao,Haoran Song,Jianhong Huang,Senlin Tian
Airborne microplastics (AMPs) and their interactions with heavy metals have attracted global concern, however, little is known about their combined effects in the lung environment. In this study, the adverse effects of polypropylene (PP, as representative AMPs)-chromium (Cr) co-exposure on natural pulmonary surfactant (PS) monolayer function was investigated. It was found that upon contact with PS, the desorption of Cr carried by inhaled PP-Cr increased and partially was (∼60 %) reduced to Cr(III). The phase behaviour of PS monolayer in co-exposure scenarios was PP dominated due to the insertion of particulates. Effects among the lipid components were observed that saturated phospholipids suffered the combined effects of Cr(VI) and Cr(III) that impaired its ability to regulate surface pressure, and unsaturated phospholipids were susceptible to infiltration by PP due to their lax structure, leading to a reduction in monolayer compressibility. Co-exposure also led to changes in lipid composition along with metabolic disturbances, and protein contained in PS tended to fold and destabilize. These findings provided front-line evidence of changes in air-liquid interface properties for PS upon PP-Cr co-exposure, suggest targets for the traceability of PS dysfunction, which is helpful for deeply understanding the unfavorable physicochemical effects of AMPs on lung health.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 1
·121009
·
IF 7.2
Wenhao Hou,Qian Xu,Yuqing Niu,Yaqi Liu,Yun Ju,Jing He,Jie Jiang,Lina Qiao,Hongbin Xie,Hong Zhang
The fine-tuning of reactions in water microdroplets remains elusive. This study demonstrated that trace amounts of positively charged inorganic salts and organic compounds promoted the C O bond reduction of oxaloacetate while inhibiting the C C bond reduction of fumarate within water microdroplets. Similar effects were observed for carbonylated molecules with varying carbon chain lengths. Unlike conventional aqueous solutions requiring millimolar dopant concentrations, dopant levels as low as 10 nM in microdroplets were sufficient to induce these selective promotion and inhibition effects. A potential mechanism involving electrostatic interactions suggested that trace positively charged dopants drove the migration of carboxylated molecules from the microdroplet surface toward its interior. This relocation correlated with the changes in reaction reactivity. These findings could offer a novel approach to mediating reaction selectivity in microdroplets and have broad implications for atmospheric chemistry, chemical synthesis, and prebiotic processes where microdroplets interact with diverse surrounding substances.
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OPTICAL MATERIALS
·
2021
·
IF 3.08
Yuyu Shen,Yi Chen,Liang Chen,Degang Deng,Shiqing Xu
An optical thermometer Bi 3+ , Eu 3+ co-doped Sr 3 La 2 Ge 3 O 12 (SLGO) phosphor with dual-emitting centers was synthesized in high-temperature condition. The X-ray diffraction patterns , SEM , EDS , luminescent properties and optical temperature sensing characteristics were exhaustive investigated. Under UV excitation, the SLGO: Bi 3+ phosphor exhibits the 3 P 1 → 1 S 0 blue luminescence of Bi 3+ peaked at 400 nm and SLGO: Eu 3+ phosphor shows the 5 D 0 → 7 F 2 red luminescence of Eu 3+ peaked at 612 nm. The ET behavior was proved by spectrum overlap between the PL spectrum of Bi 3+ and PLE spectrum of Eu 3+ . Moreover, the decay time of Bi 3+ could be verified the conclusion. Under UV excitation of 291 nm, the maximal value of absolute sensitivity ( S a ) of SLGO: Bi 3+ , Eu 3+ was 0.079 %K −1 at 573 K, and relative sensitivity ( S r ) was 0.831 %K −1 at 473 K. The results proved that SLGO: Bi 3+ , Eu 3+ phosphor could have a good performance in the field of optical thermometer.
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POWDER TECHNOLOGY
·
2019
·
IF 3.413
Aoxue Tian,Liqiong Wang,Nafeng Wang,Shuhao Wang,Jinzhi Cai,Qiao Huang,Yun Huang
Pd supported on mixed ceria-titania oxide catalysts are synthesized with a co-flow diffusion flame , and the catalytic activities for CH 4 oxidation are evaluated in a lab-scale fixed bed. The as-prepared catalysts exhibit high catalytic activities and good Pd cluster distribution. Among them, Pd supported on pure CeO 2 is found to show the best performance. The results show that it has fairly low T 10 , and complete oxidation occurs as low as 400 °C. It is deduced that three factors facilitate the reaction between the adsorbed CH 4 and O 2 , namely, solid-solution-like Pd x Ce 1- x O 2 structures, highly active sites provided by atomic-level assembly during the flame synthesis, and the presence of lattice oxygen. Additionally, the deactivation of the catalyst may be caused by the decreasing of lattice oxygen, the reduction of PdO and the instability of Pd x Ce 1- x O 2 . These results may aid in the development of better catalytic nanomaterials for clean methane oxidation .
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