APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Kai Zhu,Zhenmao Zhang,Xinyin Bai,Fangfang Chang,Qing Zhang,Ge Li,Zhengyu Bai
Electrochemical pre-reconstruction creates CuO/Cu 2 O/Cu/CeO 2 @C heterointerfaces. • Carbon confinement stabilizes multivalent Cu interfaces during CO 2 electroreduction. • CeO 2 modulates the electronic structure and interfacial charge distribution of Cu. • Reconstructed interfaces tune the thermodynamics of *CO and *OCCO formation. • Ethanol Faradaic and cathodic energy efficiencies reach 75.6% and 30.9% at −0.9 V vs. RHE. The electrochemical CO 2 reduction reaction (CO 2 RR) to ethanol provides a carbon–neutral route for the sustainable production of value-added chemicals, yet achieving high ethanol selectivity remains challenging. Herein, we report a Ce-containing Cu-based oxide precursor embedded in a carbon framework, which undergoes electrochemical pre-reconstruction to form CuO/Cu 2 O/Cu/CeO 2 @C heterostructure featuring active multi-heterointerfaces. By optimizing the Ce content, the reconstructed catalyst delivers a high ethanol Faradaic efficiency of 75.6% and an energy efficiency of 30.9% at −0.9 V versus the reversible hydrogen electrode in a flow-cell reactor, outperforming most reported Cu-based CO 2 RR electrocatalysts. Comprehensive structural characterizations reveal that the carbon confinement layer mitigates excessive reduction of Cu species and stabilizes the multivalent Cu interfacial environment during CO 2 RR, while CeO 2 modulates the local electronic structure and induces interfacial charge redistribution over Cu sites. In situ characterization combined with theoretical calculations further reveals that interfacial environment modifies the relative thermodynamics of *CO and *OCCO formation. This work provides profound insights into interfacial charge-redistribution-mediated ethanol selectivity and provides a design strategy for high-performance advanced Cu-based CO 2 RR electrocatalysts. Download: Download high-res image (80KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122907
·
IF 7.5
Xiaoyu Ma,Tao Liu,Jiaheng Huang,Jiaqi Zhang,Chengyong Yu,Tianyong Huang
Photocatalytic CO₂ reduction is a promising route for valorizing carbon resources. In liquid-phase systems, TiO 2 suffers from limited CO₂ adsorption, high interfacial charge-transfer resistance, and rapid carrier recombination. These drawbacks hinder simultaneous improvements in efficiency and selectivity. We fabricated a TiO 2 /UiO-66/Cu ternary photocatalyst using a modified-then-loaded strategy. Amino-functionalized TiO 2 was chemically anchored to UiO-66 via N–Zr coordination, forming a robust, low-resistance TiO 2 /MOF interface while preserving the CO₂-enrichment pores of UiO-66. Cu nanoparticles were then introduced as electron traps and catalytic sites to extract photogenerated electrons from the recombination-prone Type-I heterojunction, enabling directional electron utilization. In a solid–liquid system using water as the proton source, the optimal TiO 2 /UiO-66/Cu produced 86.76 μmol·g⁻¹ CO and 9.08 μmol·g⁻¹ CH 4 after 4 h of UV–visible irradiation. The CO production rate was 7.4- and 3.8-fold higher than that of pristine TiO 2 and UiO-66, respectively. Characterization shows that N–Zr coordination reduces charge-transfer resistance, UiO-66 enriches CO₂, and Cu promotes electron capture. Together, these effects mitigate the intrinsically poor charge separation of Type-I heterojunctions and enable efficient CO 2 photoreduction. The results provide design and mechanistic insights for MOF-enabled TiO 2 composite photocatalysts.
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Nature Communications
·
2026
·
IF 18.1
Qingqing Zhang,Cong Liu,Chang Xu,Dingnan Huang,Cheng Xie,Zhandong Wang,Xiao-Ming Cao,Jinlong Zhang,Juying Lei,Ziwei Ye,Lingzhi Wang
Upgrading light alkanes to value-added olefins is a long-standing challenge, owing to the high stability of C–H bonds and the tendency for overoxidation at elevated temperatures. Here, we introduce a light-driven strategy for ethane dehydrogenation using Cu-doped TiO 2 , in which atomically dispersed Cu coordinated to bridging oxygen (O br–Cu ) creates well-defined [Cu–O] ensembles that orchestrate site-specific, stepwise C–H activation. Photogenerated holes localize at O br–Cu sites to initiate the first C–H cleavage, while adjacent Cu centers mediate β–H elimination and H 2 evolution. In contrast, minor β–H activation at O br–Ti sites generates *H species that cannot desorb due to a prohibitive coupling barrier with *H on O br–Cu , leading to Cu reduction and progressive deactivation. Co-feeding CO 2 restores the active Cu coordination environment and suppresses this deactivation process without perturbing the primary reaction pathway. This cooperative design achieves a C 2 H 4 production rate of 21.1 mmol g −1 h −1 with nearly stoichiometric H 2 evolution and an apparent quantum efficiency of 6.1% under 365 nm irradiation. These findings establish a site-defined, hydrogen-conserving route for photocatalytic alkane upgrading, offering a general blueprint for selective C–H bond transformations with long-term stability. Converting light alkanes into useful olefins is hard because strong bonds and heat drive overoxidation. This study uses a copper-doped titanium dioxide photocatalyst to steer bond breaking, yielding ethylene and hydrogen.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2026
·Vol. 27
·期 5
·2486
·
IF 5.6
Liming Shi,Yuheng Liao,Zeng Hong,Jiancheng Ruan,Shaodong Zhou,Chen Wu,Chao Qian
N,N-Dimethyl-1,3-propanediamine (DMAPA) is an important aliphatic diamine widely used in fine chemical manufacturing. Its industrial production traditionally relies on Raney nickel catalysts, which suffer from pyrophoric hazards and limited selectivity due to imine condensation side reactions. To address these challenges, we report an Al2O3-supported Ni-Cu alloy catalyst as an efficient alternative for the selective hydrogenation of N,N-dimethylaminopropionitrile (DMAPN). The optimized Ni30Cu5/Al2O3catalyst achieves complete DMAPN conversion and over 90% DMAPA selectivity under industrially relevant conditions (120 °C, 2.5 MPa H2). X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy analyses confirm the formation of substitutional Ni-Cu alloy nanoparticles, where Cu incorporation induces both geometric isolation of Ni ensembles and electronic modulation of surface active sites, thereby suppressing condensation-derived by-products. In addition, an NH3/ethanol-assisted process further improves selectivity while reducing autogenous operating pressure. Overall, this work demonstrates a safe and highly selective catalytic system for primary diamine synthesis, providing a practical alternative to conventional Raney Ni-based processes.
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JOURNAL OF THE ENERGY INSTITUTE
·
2026
·
IF 6.5
Zhi-Xin Li,Hui-Jie Cheng,Yi-Han Zhang,Cong-Jian Pan,Wei-Wei Yan,Wen-Long Mo,Xiao-Qin Yang,Cai-Xia Ju,Xiao-Yu Zhang,Zhi-Hao Ma,Xian-Yong Wei,Sheng Li
Crystallinity engineering of oxide supports has emerged as a powerful strategy to enhance the performance of supported catalysts, yet its application in complex oxides like lanthanum oxycarbonate (La 2 O 2 CO 3 ) remains underexplored. Here, we demonstrated that precise control of La 2 O 2 CO 3 crystallinity via calcination temperature tuning significantly improved the reverse water-gas shift (RWGS) reaction performance of Cu-based catalysts. CuLa500 catalyst, prepared at 500 °C, exhibited superior activity and stability compared to its high-crystallinity counterpart (CuLa800, 800 °C), achieving a CO 2 conversion of 54.4% and near-unity CO selectivity (>99.9%) at 600 °C under high space velocity conditions. Systematic characterization revealed that reduced crystallinity strengthens Cu-support interactions, optimizing CO 2 adsorption while enhancing structural robustness. This work not only establishes a scalable method for RWGS catalyst optimization but also provides mechanistic insights into the role of crystallinity in complex oxide-supported systems, offering a blueprint for advancing multiphase catalysis in energy-related reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 34
·18159-18168
·
IF 3.9
Ren Xuping,Zhao Zijiang,Long Yanhui,Zhang Wenjun,Wang Jun,Zhang Hao
Developing efficient catalysts for
CO 2 hydrogenation
to methanol remains a challenge due to the inherent trade-off between
activity, selectivity, and cost. Herein, a series of metal-promoted
Cu catalysts (Zr, Zn, Ga) were synthesized via a ligand-modulated
oxalate coprecipitation strategy using malachite-derived CuO as the
precursor, enabling a low-cost and sustainable catalyst design. Among
these, the ZrO 2 /Cu catalyst (Zr/Cu = 14:86) exhibits the
optimal performance, delivering a CO 2 conversion of 13%
and a methanol space-time yield (STY) of 280.1 g MeOH ·kg cat –1 ·h –1 at 280 ° C
and 3.0 MPa, together with excellent long-term stability. Characterization
results suggest that highly dispersed Zr species effectively suppress
Cu particle agglomeration while generating abundant surface oxygen
vacancies (O V , 43.5%). Mechanistic studies indicate that
Zr incorporation induces strong electronic metal–support interactions
(EMSI), leading to the formation of electron-rich Cu 0 /Cu + sites. These sites act cooperatively with O V ,
where the former facilitates H 2 dissociation and the latter
promotes CO 2 adsorption and activation. Such synergistic
effects favor the formate-mediated pathway while suppressing the competing
reverse water–gas shift reaction. This work not only demonstrates
a high-performance catalyst derived from natural minerals but also
provides insights into the atomic-level synergy between electron-rich
metal sites and surface defects, offering a viable strategy for the
rational design of efficient catalysts for CO 2 hydrogenation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Shuai Zhang,Wen-Da Zhang,Han Zhao,Baoxin Wu,Jia-an Li,Cheng Zheng,Jiangyong Liu,Jian Wang,Jing Wang,Heng Zhao,Lin Zeng,Xiaodong Yan,Zhangxing Chen
Operando ATR-SEIRAS, DEMS, and DFT reveal an NH 2 OH-mediated AOR pathway at an enzyme-mimicking interface. • Cu 2 NCN/CuO achieves 98.93% FE at 1.50 V vs. RHE and a NO X - yield rate of 249.3 μmol cm -2 h -1 at 1.70 V vs. RHE. • A regeneration strategy mitigates surface poisoning and enables recovery of the oxidized products as crystalline KNO 3 . Electrochemical ammonia oxidation reaction (AOR) provides a promising route for the synthesis of nitrite and nitrate (termed NO x − ) under mild conditions. However, the selective conversion of NH 3 to NO x − is kinetically limited by the conventional stepwise dehydrogenation pathway. Herein, we report an ammonia monooxygenase (AMO)-inspired Cu 2 NCN/CuO heterostructure catalyst, in which the [N C–N] 2− framework provides a charge-buffering effect to stabilize Cu + -related species under oxidative AOR conditions. This biomimetic architecture enables the selective oxidation of NH 3 to NO x − by promoting a hydroxylamine (NH 2 OH)-mediated pathway that features early-stage N–O bond formation. As a result, it achieves a NO x − Faradaic efficiency as high as 98.93% at 1.50 V vs. RHE, with a corresponding yield rate of 48.48 μmol cm −2 h −1 . Operando attenuated total reflection surface-enhanced infrared absorption spectroscopy, differential electrochemical mass spectrometry, and density functional theory calculations collectively reveal that this catalytic architecture facilitates NH 2 OH intermediate formation and lowers the energy barrier for its subsequent oxidation, thereby underpinning its outstanding NO x − selectivity. These findings demonstrate that the AMO-inspired catalytic architecture provides an effective strategy for achieving efficient NO x − electrosynthesis via an NH 2 OH-mediated pathway. Download: Download high-res image (161KB) Download: Download full-size image An AMO-inspired biomimetic Cu 2 NCN/CuO heterostructure enables the selective conversion of NH 3 to NO 2 − and NO 3 − via an NH 2 OH-mediated pathway featuring early N–O bond formation.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Fen Qiao,Zaisi Zhong,Jikang Zhao,Wenjie Liu
Cu-Ni 3 S 2 /NF with varying Cu doping levels were synthesized via a two-step hydrothermal method to investigate Cu's role in enhancing Ni 3 S 2 's alkaline hydrogen evolution reaction (HER). Optimal Cu doping reduced the overpotential to 193.4 mV and Tafel slope to 87.21 mV·dec −1 at 10 mA·cm −2 in 1 M KOH, alongside achieving high conductivity and the largest electrochemical active area (910 cm 2 ). HER performance peaked then declined with excessive Cu, confirming an optimal doping threshold. DFT calculations revealed Cu modulates Ni 3 S 2 's work function and charge transport, elucidating HER enhancement mechanisms. This work provides insights for optimizing Ni 3 S 2 -based HER catalysts through controlled heteroatom doping.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jinghao Lu,Lili Yang,Chuanhui Zhang,Haijie Cao,Xingyun Li,Lianying Zhang,Chang Long,Xiu Song Zhao
Realizing the evolution of Cu valence state in the electrocatalytic CO 2 reduction reaction (eCO 2 RR) is crucial to maintain active sites, optimize reaction conditions and product selectivity and understand reaction mechanism and kinetics. In this context, we investigated the dynamic transition of Cu(II), Cu(I) and Cu(0) under the eCO 2 RR conditions and impact of such transition on reaction intermediate species and product selectivity. In situ surface-enhanced Raman spectroscopy and attenuated total reflectance-surface-enhanced infrared absorption spectroscopy results coupled with quantitative data collected from a flow cell show that Cu (I) species contributes to CO 2 activation, CO adsorption, and subsequent C–C coupling processes, while the initial adsorption of Cu (0) in CO 2 playing a crucial role. These findings clarify how the valance of Cu changes with applied cathodic potential and reaction time, thus offering guidelines on optimization of operating conditions during CO 2 electrolysis to maintain the active sites responsible for forming desirable products. These new understandings lay a solid ground for purposely designing Cu-based catalysts for improved performance in CO 2 electrolysis, significantly advancing our knowledge on the behavior of Cu-based electrocatalysts in CO 2 electrolysis.
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ACS Nano
·
2026
·
IF 16
Huafeng Fu,Shiteng Long,Jia Hu,Jiehua Li,Hansong Xue,Yu’an Chen,Fusheng Pan
To address the challenges of high hydrogen release temperatures, sluggish kinetics, and inadequate cycling performance of magnesium hydride (MgH2), we developed the niobium-based bimetallic compound catalyst CuNb2O6 with excellent catalytic performance. It was found that the MgH2/CuNb2O6 composite material achieved 4.28 wt % hydrogen uptake within 10 min at 100 °C, and even at a lower temperature of 50 °C, it has 2 wt % hydrogen absorption capacity within 60 min, showing excellent hydrogen absorption performance. For hydrogen desorption, the MgH2/CuNb2O6 composite material demonstrated exceptional midtemperature hydrogen release kinetics, with 4.65 wt % hydrogen released within 20 min at 225 °C. The apparent activation energy for hydrogen release of MgH2/CuNb2O6 was determined to be 50.95 kJ/mol, which was approximately 66.4% less than that of ball-milled magnesium hydride. Cyclic testing further confirmed the stability of the MgH2/CuNb2O6 composite, with its hydrogen storage capacity stabilizing at 5.21 wt % after 50 cycles. Catalytic mechanism studies revealed that the MgH2/CuNb2O6 composite undergoes in situ reconstruction of multiple-phase catalytically active species, which effectively improved the hydrogen storage performance of MgH2. This work innovatively constructed a representative Mg2Cu@NbO2 heterojunction, and the results showed that hydrogen molecules were significantly activated at the interface, demonstrating the synergistic catalytic effect between the Cu and Nb species. This study provides a possible approach for designing high-efficiency catalysts for magnesium-based hydrogen storage materials.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.7
Yarong Chai,Bo Gao,Song Xu,Qun Xu
Electrocatalytic conversion of nitrate to ammonia is a rapidly evolving field due to its potential applications toward nitrate pollution remediation and sustainable ammonia synthesis. As a group of well-established electrocatalysts, the activity of Cu-based materials is highly related to the coordination environment. Herein, a novel Cu–La-based dual-atom catalyst (Cu–La/DAC) was prepared using a Robson-type bimetallic Cu–La complex as precursor, where the square-planar Cu center of Cu–La/DAC effectively deviates due to the presence of adjacent La atom. As a result, the HOMO (dxy) energy of Cu is effectively reduced, which facilitates the formation of low-valent Cu and subsequent electrocatalysis. Compared to Cu2/DAC analogue containing square-planar Cu, Cu–La/DAC exhibits significantly enhanced activity toward electrocatalytic nitrate (NO3–) reduction to ammonia (NH3) (yield: 14.02 mg h–1 cm–2; Faraday efficiency: 88.42%), which is theoretically attributed to the reduced energy barrier of NO3– adsorption and *NO3 deoxygenation induced upon the coordination environment modulation of Cu.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 11
·1-9
·
IF 5.7
Deng Yan,Li Shuhuai,Ma Xionghui,Wu Yuwei,Pang Chaohai,Wang Mingyue,Li Jianping,Zhi Xu
The key to developing sensors for chiral drug determination is to exclude interference from enantiomers. In this study, metal–organic frameworks (MOFs) and molecularly imprinted polymer (MIP) were introduced to prepare a chiral sensor for levofloxacin detection. The MIP was electropolymerised on the surface of the Cu/Fe-benzene-1,3,5-tricarboxylate MOF (Cu/Fe-BTC)-modified Au electrode using levofloxacin as a template molecule. After eluting the levofloxacin, a chiral sensor with recognition sites for levofloxacin was obtained. With this site as a switch, a novel method for detecting levofloxacin was established. Because of the enhanced recognition effect, the sensor can effectively exclude the enantiomeric interference of d-ofloxacin. Moreover, Cu/Fe-BTC can effectively amplify the current response signal and improve the sensitivity of the sensor. The linear range of the sensor was 5 to 4000 × 10 −11 mol L −1 , and the detection limit was 2.07 × 10 −11 mol L −1 . When applied to detecting levofloxacin in actual samples, the sensor showed a 92.7–109.8% recovery. Graphical
研究领域:
分析化学
·
药物分析
·
材料科学
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