iScience
·
2026
·Vol. 29
·期 6
·
IF 4.5
Ziyu Wang,Xuejie Han,Baohao Qian,Xiulai Zhang,Jingyuan Ma,Ru Feng,Meiqin Shi,Guangbo Chen,Fanfei Sun
Photothermal catalytic reduction of CO 2 to CO has been regarded as a promising strategy for solar-to-chemical energy conversion, yet the dynamic evolution of active sites under realistic reaction conditions remains poorly understood. Herein, we synthesized CuO/ZnO (CuZnO) catalysts with intimate interfacial contact via co-precipitation followed by calcination method. Under photothermal conditions, CuZnO underwent in situ reconstruction into low-coordinated metallic Cu in close contact with ZnO, delivering a CO generation rate of ∼18.1 mmol g −1 h −1 with a selectivity as high as 99% at 200 °C, outperforming that achieved under purely thermal conditions. Operando photothermal X-ray absorption fine structure (XAFS) spectroscopy revealed the real-time evolution of both Cu and Zn coordination environments in CuZnO, illustrating the formation and stabilization of metallic Cu on ZnO during photothermal catalysis. This study elucidates the mechanisms underlying photothermal synergy in CO 2 reduction and provides mechanistic insights into active-site dynamics under photothermal conditions.
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Molecular Catalysis
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2026
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IF 4.3
Hanyue Xiao,Shasha Zhao,Kai Peng,Yaoyao Xu,Juan Li,Bodun Xie,Yao Si,Guowei Deng,Min Yang,Wei Li
In 1 M KOH, at 10 mA·cm⁻², the overpotential of HER is as low as 60.6 mV, and the Tafel slope is 90.07 mV·dec⁻¹. • At 100 mA·cm⁻², in 0.5 M H 2 SO 4 , the overpotential of OER is only 247.3 mV. After 300 h, the current density remains at 94.8%, and the voltage for overall water splitting is as low as 1.07 V. • CuRu@NF-AC exhibits excellent water splitting performance over the entire pH range, with the Faraday efficiencies of HER and OER reaching as high as 99.73% and 99.87%, respectively. In response to the energy crisis and environmental issues, to address the shortcomings of traditional electrocatalytic materials such as insufficient activity and poor stability, this study innovatively synthesized CuRu@NF-AC nanomaterials through an interface regulation strategy and systematically investigated their performance in electrocatalytic water splitting (hydrogen evolution reaction (HER) and oxygen evolution reaction (OER)) across the entire pH range. Experimental results demonstrate that this material achieves significant electrocatalytic activity through interface structure optimization. At a current density of 10 mA·cm −2 , the overpotentials for OER and HER in alkaline conditions were as low as 44.4 mV and 60.6 mV, respectively, with Tafel slopes of 30.14 mV·dec⁻¹ and 90.07 mV·dec⁻¹. In acidic conditions, the OER excess potential is only 49 mV and the overall water splitting voltage is as low as 1.07 V. In neutral (1.0 M PBS) electrolyte, the HER overpotential is 302.6 mV at 10 mA·cm −2 with a Tafel slope of 76.25 mV·dec⁻¹, exhibiting superior pH-universal adaptability. In addition, the catalyst exhibits excellent long-term stability, maintaining a stable electrocatalytic performance for >100 h. This study provides a new strategy for designing pH-universal hydrogen evolution electrocatalysts via interface regulation, with important theoretical and practical value. Download: Download high-res image (417KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
·
IF 9.6
Donghai Wu,Silu Li,Guanghua Lu,Hanyu Fang,Jun Hou
Co 0.5 /Cu 0.5 -Ti 3 C 2 Tₓ achieved excellent PMS activation and APAP removal. • A synergistic radical/non-radical mechanism governed the efficient degradation process. • Co/Cu diatomic synergy enhanced PMS adsorption, electron transfer, and mutual redox cycling. • APAP degradation pathways were elucidated, confirming effective detoxification. A central challenge in heterogeneous peroxymonosulfate (PMS) activation is achieving catalysts with highly active interfacial sites to enable both efficient pollutant degradation and environmentally safe water treatment. Herein, cooperative Co/Cu dual-atom sites were anchored on Ti 3 C 2 T x MXene (Co/Cu-Ti 3 C 2 T x ). The optimized Co 0.5 /Cu 0.5 -Ti 3 C 2 T x catalyst achieved 96.9% removal of the emerging contaminant acetaminophen (APAP) within 60 min via PMS activation, markedly outperforming its single-atom analogues by 21.0–58.6%. Response surface methodology (RSM) analysis indicated that the system operated efficiently under near-neutral pH and mild conditions. Quenching experiments and electron paramagnetic resonance (EPR) analysis suggested that APAP degradation proceeded via a coupled mechanism involving contributions from both reactive oxygen species (predominantly •OH, •O 2 − , and 1 O 2 ) and high-valent metal-oxo species (HVMOS). Density functional theory (DFT) calculations revealed that the synergistic interaction between Co/Cu sites enhanced PMS adsorption, improved electron transfer efficiency, and accelerated the redox cycles between Co 0 /Co 2+ and Cu + /Cu 2+ , thereby cooperatively promoting the activation of PMS. Based on the identification of intermediates, the degradation pathway of APAP was proposed to involve hydroxylation of the benzene ring, ring-opening, deacetylation, and ultimately oxidative degradation. The biotoxicity of the treated effluent decreased, confirming the effectiveness and environmental safety of the process. These findings advance the mechanistic understanding of bimetallic PMS activation and present a viable approach for the remediation of water containing refractory emerging contaminants. Download: Download high-res image (148KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122789
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IF 7.5
Dancheng Zhu,Caiyun Zhang,Jiabin Shen,Chao Shen,Chuanhong Jin,Hao Xu
Sulfamethoxazole (SMX), a widely used sulfonamide antibiotic, is a persistent aquatic pollutant due to its resistance to conventional treatment. Here, a Cu-ZSM-5/Ti 3 C 2 composite catalyst was fabricated by electrostatic self-assembly for peroxymonosulfate (PMS) activation. Characterization by XRD, SEM, TEM, XPS, and zeta potential analysis confirmed the successful integration of the components. The catalyst achieved 97.59% removal of 10 mg/L SMX within 30 min. Quenching and EPR results indicated that 1 O 2 was the major reactive species. The enhanced performance under alkaline conditions was associated with the negatively charged composite surface (-38.8 mV at pH 9), the deprotonated state of SMX, and favorable interfacial interactions that may promote preferential oxidation of the isoxazole moiety. Control experiments using a physically mixed sample showed markedly lower activity, especially at pH 11, highlighting the importance of the intimate heterointerface created by self-assembly. The superior activity was attributed to the synergistic interaction between Cu species in Cu-ZSM-5 and Ti-based sites in Ti 3 C 2 . This work provides insight into designing selective PMS activation catalysts for antibiotic-contaminated water treatment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Yan Chen,Chao Lei,Kun Yang,Ming-Li Ye,Yong-Gang Zhao,Yun Zhang
Metal organic frameworks (MOFs) are widely employed as separable and highly efficient adsorbents in VOCs (volatile organic compounds) pollution in the air. However, due to poor stability and easy hydrolysis in water, traditional MOFs cannot yet be used for the removal of VOCs in wastewater. Here, a novel series of magnetic Fe–Cu bimetallic MOFs possessing dual hydrophilic and hydrophobic functionality was prepared for VOCs removal in wastewater. The materials were characterized using scanning electron microscopy (SEM), vibrating sample magnetometry (VSM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results indicate that both of the morphological and adsorption performance of magnetic Fe–Cu bimetallic MOFs are highly dependent on the molar ratio of ethylenediamine to 4,4-bipyridine used during synthesis. When the molar ratios of ethylenediamine to 4,4-bipyridine are 5:1, 1:1, and 1:5, the morphologies of prepared magnetic Fe–Cu bimetallic MOFs are gravel-like, cobble-like and calcite-like, respectively. They are named as magnetic gravel-like Fe–Cu metal organic frameworks (Mag-Gra-Fe-Cu MOFs), magnetic cobble-like Fe–Cu metal organic frameworks (Mag-CoL-Fe-Cu MOFs) and calcite-like Fe–Cu metal organic frameworks (Mag-CaL-Fe-Cu MOFs). Moreover, the maximum adsorption capacity of Mag-Gra-Fe-Cu MOFs, Mag-CoL-Fe-Cu MOFs and Mag-CaL-Fe-Cu MOFs could reach up to 487.80–621.12 mg/g, 549.45–666.67 mg/g and 598.80–724.64 mg/g, respectively. Under optimal conditions, the adsorption of VOCs onto the magnetic Fe–Cu bimetallic MOFs followed the pseudo-second-order kinetic model (R² = 1) and the Langmuir isotherm model (R² > 0.999). Consequently, the magnetic Fe–Cu bimetallic MOFs developed in this work represent a viable and efficient option for removing VOCs from wastewater. Download: Download high-res image (251KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Wenda Chen,Shenghua Ye,Wei Zeng,Xin Wang,Yixiao Zou,Peng Cui,Kang Liao,Lirong Zheng,Yantong Xu,Qianling Zhang,Xiaopeng Han,Wenbin Hu
1,4-benzenedicarboxylate-modified Cu nanosheets were synthesized via 2D Cu-BDC MOF precursor and template. • Carboxyl groups on Cu surface enhance H 2 O accumulation for sustained proton supply. • Carboxylate-mediated proton transfer accelerates *NO → *NOH. Tailoring the interfacial microenvironment is essential for regulating proton-coupled electron transfer (PCET) dynamics, key processes governing the electrochemical nitrate reduction reaction (NO 3 − RR) for efficient ammonia (NH 3 ) synthesis. Herein, we design a metal-organic framework-derived Cu nanosheet architecture modified with 1,4-benzenedicarboxylate (BDC@Cu NSs), where BDC molecules serve as built-in “proton pumps” to boost electrocatalytic NO 3 − RR with higher NH 3 production. In situ spectroscopic characterizations, kinetic isotope effect measurements and theoretical calculations demonstrate that the carboxylate groups (−COO − ) of BDC 2− adsorbed on the Cu interface construct an enhanced interfacial hydrogen-bond network for facilitating H 2 O accumulation and dissociation, and capture and transfer protons to nitrogen-containing intermediates via a PCET pathway, which drastically lowers the energy barrier of the potential-determining step (*NO hydrogenation to *NOH), endowing BDC@Cu NSs with a high NH 3 yield, superior Faradaic efficiency, and outstanding operational durability. This study presents a design strategy for engineering electrocatalytic interfacial microenvironments and provides fundamental insight into proton transport within hydrogen-bonded networks at the interface. Download: Download high-res image (136KB) Download: Download full-size image Constructing built-in proton pumps on MOF-derived Cu nanosheets via surface-anchored carboxylate groups enables efficient electrocatalytic nitrate reduction. These groups establish an enhanced interfacial hydrogen-bond network, facilitating H 2 O dissociation and selective proton transfer to *NO intermediates, thereby drastically lowers the energy barrier for ammonia synthesis.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2026
·
IF 3.1
He Shuangyi,Zhao Weiwei,Zhang Shuai,Li Tianbao,Luo Jujie
Cu − Bi bimetallic material with excellent electrochemical performance was successfully fabricated on iron foam via a one-stop microwave method. Under the optimal microwave power, heating time, and metal molar ratio, metallic Bi presents a needle-like morphology, interconnects to form a network, and is coated with Bi. This unique structure endows the Cu − Bi bimetal with the best electrochemical performance. Meanwhile, metallic Fe undergoes redox reactions in the alkaline electrolyte, which further enhances the capacitance value. The electrode prepared under the optimal synthesis conditions achieves an impressive areal capacitance value of 7.55 F cm −2 when tested at 1 A cm −2 , and it maintains 77.47% of its initially measured capacitance even after undergoing 15,000 long-term charge–discharge cycles, demonstrating excellent electrochemical stability. The assembled asymmetric supercapacitor device retains 84.1% of its original capacitance after 20,000 cycles. A power density value of 1185 μW cm −2 is realized when the energy density reaches 766.96 μWh cm −2 .
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ACS Applied Materials & Interfaces
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2026
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IF 7.8
Dewen Fu,Guoju Wang,Zhifeng Zhang,Zhiqiang Wu,Xuemei Zhang,Wenfei Dong
Ammonia, as a crucial feedstock in the chemical industry, is traditionally synthesized via the energy-intensive and high-carbon-emission Haber–Bosch process, which contradicts sustainable development goals. The electrocatalytic nitrate reduction reaction (NO3RR) for ammonia synthesis has emerged as a research hotspot due to its low energy consumption and environmental friendliness. However, existing catalysts still suffer from high overpotentials, competitive hydrogen evolution reaction (HER), and intermediate accumulation. In this study, we successfully fabricated copper-doped cobalt phosphide (Cu-CoP) catalysts through hydrothermal and phosphidation strategies, systematically investigating their NO3RR performance and mechanism. Experimental results demonstrate that Cu-CoP exhibits exceptional catalytic activity at −0.65 V vs RHE, achieving a Faradaic efficiency of 96.2% and an ammonia production rate of 7.06 mg cm–2 h–1, significantly outperforming undoped CoP catalysts. Through comprehensive characterization and theoretical calculations, we reveal that Cu incorporation not only optimizes the electronic structure of Co sites to facilitate water dissociation and *H generation, but also enables efficient nitrate adsorption at Cu sites while suppressing *H dimerization, thereby synergistically enhancing NO3RR selectivity and kinetics. This work provides insights for designing high-performance nonprecious metal NO3RR catalysts and elucidates the cooperative mechanism of dual active sites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
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IF 9.6
Ziwen Feng,Di Liu,Jiaqian Kang,Chunfa Liu,Lun Li,Juanjuan Wang,Zhenyu Zhang,Xingyou Li,Weng Fai Ip,Hui Pan
Identifying the true active sites is essential for the development of efficient catalysts for the electrochemical reduction of neutral, dilute nitrate to ammonia, because electrocatalysts often undergo structural transformations during operation conditions, potentially forming new active phases. In this work, copper oxides nanowires with varying Cu valence states were fabricated by in-situ electrochemical reduction of the pre-catalysts (denoted as P-CuO 200, CuO 300, and CuO 400 ) for the electrochemical reduction of neutral, dilute nitrate (5 mM) to ammonia. In-situ and ex-situ characterizations indicated that the surface CuO of these pre-catalysts was partially or fully reduced to Cu 2 O or metallic Cu during activation process. The Cu 2 O species were further transformed into oxide-derived copper (OD-Cu), serving as the true active sites. Among them, the CuO 300 (OD-Cu/Cu 2 O) catalyst with the highest Cu 2 O content, achieved a Faradaic efficiency of 90.8%, a nitrate conversion of 98.3%, and an ammonia yield of 3.3 mg h −1 cm −2 at −0.4 V vs. RHE, outperforming most reported Cu-based materials. Computational results confirmed that OD-Cu facilitated *NO 2 adsorption and protonation, lowering the energy barrier. This study bridges the critical gap between pre-catalyst structures and dynamically formed active sites, providing valuable guidance for the rational design of Cu-based catalysts. Download: Download high-res image (101KB) Download: Download full-size image
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WATER RESEARCH
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2026
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IF 12.8
Yifei Peng,Ruya Chen,Zhuoya Fang,Xinyuan Qiu,Qingzhen Wang,Huajun Feng,Jinming Luo,Yijing Xia
Sulfur-mediated electroreduction provides an attractive route for the concurrent decomplexation and recovery of persistent Cu(II)-EDTA; however, the intrinsic activity of sulfur sites remains poorly defined. Here, MoS 2 is employed as a model platform to delineate the role of sulfur functionalities by comparing the metallic 1T and semiconducting 2H phases. Studies reveal that sulfur sites promote a direct two-electron reduction pathway from Cu(II) to Cu(0). In the 1T phase, enhanced covalent Cu-S interactions lower the adsorption and activation barriers of Cu(II)-EDTA, while the elevated density of states at the Fermi level facilitates rapid electron transfer. Combined spectroscopic and theoretical analyses further show that sulfur vacancies and distorted octahedral coordination in 1T-MoS 2 modulate the electronic structure of sulfur sites, thereby promoting Cu extraction and lowering the decomplexation barrier. Consequently, 1T-MoS 2 achieves 99.4% Cu recovery with > 99% EDTA preservation, corresponding to an energy efficiency of 198.80 g kWh -1 (at an initial concentration of 100 mg L -1 ), outperforming 2H-MoS 2 (82.85%, 153.43 g kWh -1 ). This sulfur-mediated pathway concurrently enables stable operation over 30 cycles with high selectivity in complex matrices. Moreover, the strategy extends to other metal-EDTA systems ( e.g. , Pb(II), Cd(II)), highlighting the generality of sulfur-active electrocatalysts for coupling ligand preservation with efficient heavy-metal recovery.
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RSC Advances
·
2026
·Vol. 16
·期 18
·16748-16755
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IF 6.1
Yuqi Zhang,Yuan Yao,Peihao Dou,Qing Cheng,Yanqiang Zhang
An ionic liquid (IL)-H2O2 propellant offers a green alternative to the traditional hydrazine-N2O4 system. Due to the weak oxidizing ability of H2O2, typical ILs cannot be spontaneously ignited. To address this issue, catalytic ignition was proposed, and a series of metal complex catalysts with the formula M(vim)2(DCA)2 (M = Mn, Fe, Co, and Cu) were synthesized. Single-crystal X-ray diffraction analysis shows that the Mn, Fe and Co complexes adopt an octahedral geometry, while the Cu complex exhibits a planar quadrilateral geometry. The physicochemical properties (Td, ΔHc, ΔHf, and Isp) of the fuels (10 wt% M(vim)2(DCA)2 + 90 wt% [BMIM]DCA) were evaluated. Dynamic light scattering and UV-vis spectroscopy analyses confirm that the four complexes disperse well in [BMIM]DCA. Ignition tests reveal that Cu(vim)2(DCA)2 exhibits the best catalytic performance for the ignition of [BMIM]DCA with H2O2, achieving tid as short as 21 ms. EPR studies indicate that Cu(vim)2(DCA)2 catalyzes H2O2 to generate reactive oxygen species (·OH, ·O2−, and 1O2), which subsequently induce the spontaneous ignition of [BMIM]DCA. DFT calculations reveal that the zero-dimensional geometry of Cu(vim)2(DCA)2 features an unsaturated Cu center and electron-rich ligand framework. This typical structure enables efficient electron transfer to activate H2O2, boosting ROS generation and ignition. This work clarifies the crucial role of the metal center in the IL-H2O2 system and provides an important insight into the catalytic ignition of the “double-green” propellants.
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MICROCHEMICAL JOURNAL
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2026
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IF 5.2
Li Wang,Liwei Wang,Yuhang Que,Ling Xin,Fugang Xu
Donut-like Cu-Zn-MOF@CuNPs were synthesized via facile two-step approaches. • Cl − amplifies Cu signal via formation of highly electroactive CuCl. • Ag + inhibits the signal by competitive binding with Cl − to form AgCl. • The sensor detects Ag + with a low LOD of 1.4 nM and wide linear range. • It shows good selectivity, stability, and real water sample recovery. Silver ions (Ag + ) are highly toxic heavy metal pollutants. Conventional electrochemical methods for Ag + detection typically involve complex ionophore preparation, long preconcentration/stripping steps, or costly biorecognition agent. Here, we report a Cu-Zn-MOF supported CuNPs composite (Cu-Zn-MOF/CuNPs) for Ag + detection. The composite is prepared via a two-step room temperature mixing process. The nest-like Cu-Zn-MOF, composed of stacked two-dimensional nanosheets, provides a high specific surface area and accessible active sites for CuNPs deposition, which improves conductivity and generates a detectable redox signal. The presence of Cl − enhances the Cu redox signal due to the formation of electroactive CuCl. In the presence of Ag + , this signal enhancement is suppressed due to the competitive binding that forms AgCl precipitates. Leveraging this “amplification-inhibition” response, the Cu-Zn-MOF/CuNPs modified electrode allows for Ag + detection with two linear ranges (5 nM–100 nM and 100 nM–1100 nM), a detection limit of 1.4 nM, and recoveries ranging from 96.5% to 104.5% in spiked real water samples. The preparation procedure and detection protocol are relatively straightforward, and the sensing mechanism offers an alternative pathway for heavy metal ion detection. A donut-like Cu-Zn-MOF/CuNPs composite enables sensitive and selective electrochemical detection of Ag + via a novel amplification-inhibition mechanism: Cl − enhances the Cu redox signal through CuCl formation, while Ag + competitively binds Cl − to suppress the signal. The sensor achieves a low detection limit of 1.4 nM and good performance in real water samples. Download: Download high-res image (121KB) Download: Download full-size image
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