CATALYSIS LETTERS
·
2026
·Vol. 156
·期 8
·229
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IF 2.5
Sun Zeyun,Wang Jiapan,Pu Weijia,Liu Yang,Xiao Yahui,Pu Yanfeng,Zhao Junwei,Liu Yong
The hydrogenation of esters to corresponding alcohols is a crucial yet challenging process in sustainable chemistry, demanding efficient and stable non-noble metal catalysts. In this study, a CuZnO x /CeO 2 metal-oxide catalyst was synthesized via a metal-organic framework (MOF)-derived route for the hydrogenation of cyclohexyl acetate. The catalyst, featuring highly dispersed Cu species and low Cu loading (11.4wt%), was obtained by calcining a Ce-MOF precursor incorporated with Cu and Zn. By modulating the reduction temperature, the mixed valence state Cu 0 and Cu + active species were observed to coexist on the catalyst surface. After systematic investigation of structure-activity relationship in catalytic hydrogenation, and the optimized CuZnO x /CeO 2 -400-350 catalyst reached 99.9% conversion of cyclohexyl acetate, with selectivity of 98.2% to cyclohexanol under mild conditions (240 °C, 3 MPa H 2 , 11.4 wt% Cu loading in actual, 4 h). Moreover, it exhibited outstanding recyclability, maintaining over 99.0% conversion and above 97.0% cyclohexanol selectivity after five cycles. XRD and XPS analyses revealed no significant changes in the crystal structure or Cu 0 /Cu + species after reaction, confirming excellent resistance to sintering and remarkable structural stability. This work affords a feasible way for designing high-performance catalysts for ester hydrogenation, demonstrating significant potential for industrial application. Graphical
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Lei Guo,Gaobo Lin,Jie Zhu,Wenhua Zhou,Jiaji Zhang,Weiyu Song,Jianghao Wang,Jie Fu
Substituting the oxygen evolution reaction with formaldehyde oxidation in aqueous electrochemical systems can simultaneously reduce energy consumption and yield value-added products such as hydrogen and formic acid. However, Cu-based catalysts suffer from oxidative deactivation, limiting their electrochemical window (<0.6 V) and compromising activity and stability. Herein, a dynamic self-stabilization strategy for formaldehyde electrooxidation at high potentials, where high-coverage HCHO species stabilizes Cu 0/+ catalysts to sustain continuous catalysis, is proposed. This approach extends the reaction potential window beyond 1 V, achieving ampere-level current densities. Quasi-in-situ Raman spectroscopy and in situ X-ray absorption spectroscopy confirm Cu 0 as the primary active site across a broad potential range. In situ infrared spectroscopy and density functional theory calculations reveal that the Cu + enhances formaldehyde adsorption at high potentials while suppressing excessive OH − coverage, mitigating oxidative deactivation and boosting catalyst stability. Moreover, using this Cu 0/+ electrocatalyst, this study develops a non-noble-metal-based bipolar hydrogen production device, delivering 10 A at 0.6 V with near-unity Faradaic efficiency for both hydrogen and formate production. This work offers a robust framework for expanding the redox potential window of organic molecule electrooxidation.
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APPLIED CATALYSIS A-GENERAL
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2025
·
IF 4.8
Can Zhu,Yuehui Luo,Wanyun Tang,Nan Huang,Shiju Tao,Huan Yang,Hao Feng,Quanxin Li
The high value transformation of renewable lignocellulose is crucial for reducing carbon emissions and promoting sustainable development. This effort aims to demonstrate that bio-based cresol (an important high-value chemical) can be yielded from lignocellulosic biomass. This novel directed conversion was effectuated by coupling catalytic pyrolysis of lignocellulose into aromatic intermediates and catalytic hydroxylation of aromatic intermediates into bio-based cresol. We also developed a highly active and recyclable magnetic catalyst (Cu 0 -CuFe 2 O 4 @Biochar(HTR)), confirming that introducing Cu 0 into the copper-iron composite metal oxide catalyst promotes hydroxyl radicals formation and the synthesis of bio-based cresol. The Cu 0 -CuFe 2 O 4 @Biochar(HTR) catalyst exhibited high cresol selectivity (81.1 %) and high cresol yield (54.3 %) in catalytic hydroxylation of aromatic intermediates into bio-based cresol. Based on catalyst characterizations and hydroxyl radicals analysis, the presumable reaction mechanism related to the bio-based cresol synthesis was proposed. Potentially, this strategy may provide a beneficial pathway for developing high-value bio-based chemical (cresol) using renewable lignocellulosic biomass.
研究领域:
催化化学
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可再生能源
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绿色化学
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生物质转化
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材料科学
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Li Zeyu,Zheng Ming,Yan Chunshuang,Yang Dongqi,Yang Ruyu,Zhang Chu,Liu Hengjie,Song Pin,Yin Chenhui,Qi Zeming,Liu Daobin,Zhou Xin,Song Li,Lv Chade,Yu Guihua
The synergistic Cu 0 -Cu δ+ sites are found as the active sites for NH 3 synthesis through nitrate electroreduction reaction, but still face significant challenges in stabilizing the Cu δ+ due to its self-reduction. Here we propose an Ohmic contact interface engineering strategy by loading copper nano-islands on indium hydroxide nanocubes. Attributed to the lower work function of Cu than that of In(OH) 3 with n-type semiconductor nature, the electrons in Cu can transfer unimpededly to In(OH) 3 at the interface of Ohmic junction, triggering and stabilizing polarized Cu 0 -Cu δ+ active sites. Cu@In(OH) 3 sustains both high NH 3 yield rate (4.28 mmol h −1 mg cat. −1 ) and Faradaic efficiency (97.35%) at −0.6 V vs. RHE, while maintaining stability for at least 120 h under an Ampere-level of 800 mA cm −2 . Such Ohmic contact interface engineering approach allows for simultaneously constructing and stabilizing the Cu 0 -Cu δ+ for the electrosynthesis of ammonia, as well as other value-added chemicals relying on above active sites.
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Nano Energy
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2023
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IF 17.6
Hao Zhang,Ying Wang.,Qiong Lei,Ying Wang,Chiu Tang,Jun Yin,Tsz Woon Benedict Lo
Tracking the evolution of electrocatalysts over oxide-derived Cu materials during the electrochemical CO 2 reduction reaction (eCO 2 RR) is pivotal for optimizing the product selectivity toward desired multi-carbon (C 2+ ) products. However, the identification of the true intermediate active catalyst is still unclear. Here, we adopted a multi-modal characterization approach, primarily based on operando powder X-ray diffraction and operando micro-Raman spectroscopy, to study three Cu 2 O precursors with different morphologies, namely, octahedral (O-), cubic (C-), and nanowire (N-Cu 2 O). This multi-modal approach allows us to investigate the Cu 2 O nano-crystallites from the interface to the bulk structure. The results suggested notably different electrochemical reduction kinetics. 26.1% O-Cu 2 O and 90.6% C-Cu 2 O were reduced to much smaller Cu(0) domains after two hours of time-on-stream; N-Cu 2 O, with notably higher surface-to-volume ratio, was completely reduced within 45 min of time-on-stream. We accordingly observed a structure-reactivity correlation where a more intricate Cu 2 O/Cu grain network (and hence Cu + -Cu 0 junctions) as observed in O-Cu 2 O, can lead to stable and quantitative production of ethylene at the Faradic efficiency of around 40% (in stark contrast to those of C- and N-Cu 2 O). The synergy between the Cu 2 O and Cu phases was also verified by density functional theory calculations. The upshifted d -band center of Cu 2 O/Cu in O-Cu 2 O is the most conducive toward the production of ethylene, whereas the downshifted d -band center of Cu 2 O/Cu in C-Cu 2 O leads to a decreased production of ethylene in the expense of unwanted production of hydrogen. We envisage that system optimization and design of new catalysts will become more facile and efficient using a related multi-modal operando characterization philosophy.
研究领域:
材料科学
·
电化学
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Longqian Xu,Kaili Yan,Yunfeng Mao,Deli Wu
Using copper and/or iron based nanomaterial to activate dioxygen to produce free radicals is an alternative and environmental friendly technique, but the low conversion efficiency of oxygen and the rate-limiting step of superoxide radical generation limit current application. In present work, Cu 0 nano-shell-decorated nZVI (CFNs) was synthesized and employed to enhance the activation of oxygen for the removal of arsenic at circumneutral pH. The adsorption and oxidation pathways of arsenic were investigated by determination of arsenic distribution and radical scavenger methods. The results showed that the removal of arsenic by CFNs involved the initial step of As III adsorption by ferrihydrite followed by the oxidation of As III by hydroxyl radical ( OH abs ) and superoxide radical ( O 2 − abs ) radicals. In the presence of oxygen, the removal capacity of CFNs was improved twice than that of conventional nZVI (i.e. 453 mg/g and 263 mg/g, respectively). We inferred that Cu I in-situ generated in heterogeneous catalysis was of increasing importance and the O 2 – abs produced from the activation of dioxygen was regarded as the key factor in the generation of H 2 O 2 at pH 7. The enhancement of Cu I generation mainly because of: (i) the facial loading of Cu 0 shell accelerated the generation of Cu I , (ii) reductive Fe 0 core contributed to the regeneration of Cu I , and (iii) the generation of ferrihydrite with high specific surface area favored the adsorption of oxygen. Hence, CFNs enhanced the electron transfer between Cu I /Fe II and O 2 , increased the utilization efficiency of oxidants and improved the effectiveness of the functional nanoparticles for environmental applications.
研究领域:
环境科学
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纳米材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Duxia Li,Mingkun Wu,Zunqing Lou,Mengkui Tian
Volatile radioactive iodine from the nuclear industry poses persistent safety risks, thus making it critical to develop adsorbents for efficient capture of elemental iodine in both gaseous and liquid phases. Ti 3 C 2 T x MXene is a promising environmental adsorbent, but its iodine adsorption performance is limited by scarce intrinsic high-activity metal sites. Existing MXene-based adsorbents mostly rely on fluorine-containing etching or silver loading, suffering from fluorine toxicity and potential biotoxicity. Most only focus on single-phase adsorption, and few study their adsorption performance in both gas and liquid phases. The atomic-level synergistic mechanism remains unclear. In this work, a green Lewis acid molten salt etching method was used to prepare highly dispersed Cu 0 -loaded MXene via one-step in situ synthesis, using copper chloride as both etchant and copper source. Notably, a fluorine-free in-situ etched Cu-based MXene is developed herein and applied to elemental iodine capture in both gaseous and liquid phases. Its adsorption capacities reached 1525.33 mg·g −1 (liquid, 45 °C) and 1190 mg·g −1 (gas, 200 °C), outperforming Ti 3 AlC 2 precursor, pristine MXene and most reported modified MXene materials and commercial silver-loaded zeolites. Dynamic breakthrough tests yield a saturation capacity of 726 mg·g −1 under 150 ppmv iodine vapor (20 sccm), with 582 mg·g −1 retained under 400 ppmv CO 2 competition. For 150 °C static gaseous adsorption, the adsorbent maintains 83.22% of its initial capacity after 5 regeneration cycles and 72.65% after 6 cycles via sodium borohydride elution. Systematic characterizations and DFT calculations confirmed efficient iodine immobilization via a physicochemical synergistic mechanism: chemisorption dominated by Cu 0 Ti dual active sites forming stable CuI and Ti I bonds, supplemented by interlayer physisorption. This work provides new insights into the green design of high-performance iodine adsorbents and atomic-level mechanism elucidation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Yunqing Zhu,Sixiang Mao,Tian Wang,Fan Pan,Kejing Zhang,Shanshan Yu,Chuanyi Wang
Electrochemical nitrate reduction reaction (eNO 3 RR) technology offers a sustainable approach for ammonia synthesis due to its high efficiency and environmental compatibility. However, the complex multi-electron reduction process limits catalytic activity and selectivity. Herein, a tandem catalytic system is designed to address this challenge. A Cu 0 /P 2 Mo 18 /CF composite electrode, featuring copper (Cu) nanoparticle- modified P 2 Mo 18 nanocolumns, was prepared via one-step hydrothermal synthesis. The as-fabricated electrode delivers outstanding electrocatalytic performance toward eNO 3 RR. At a potential of −0.7 V vs. RHE, the nitrate (NO 3 − ) removal efficiency and ammonia (NH 3 ) selectivity reach 99% and 91%, respectively, alongside a high NH 3 yield of 666.6 μg·h −1 ·cm −2 . Moreover, the electrode retains superior catalytic activity and stability after 30 consecutive cyclic tests. The superior performance stems from the cascade effect between Cu 0 /Cu + on copper nanoparticles and P 2 Mo 18 . Cu 0 /Cu + facilitates rapid NO 3 − adsorption and reduction to nitrite (NO 2 − ), while electron-rich [P 2 Mo 18 O 62 ] 6− and acidic sites selectively reduce intermediates to NH 3 . In situ characterization further reveals that the reaction pathway proceeds as follows: *NO 3 − → *NO 2 − → *NO→*N → *NH → *NH 2 → *NH 3 . This work establishes a polyoxometalate-based cascade catalytic system, providing a novel strategy for designing efficient electrocatalysts for selective nitrate-to-ammonia conversion.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yue Chen,Yu Ma,Chen Liao,Jiacheng You,Huihuang Fang,Chongqi Chen,Yu Luo,Lilong Jiang
The construction and stabilization of Cu–O–Si interfaces in copper-based catalysts remain critical yet challenging for the water-gas shift reaction (WGSR), as conventional strategies fail to mitigate copper nanoparticle (NP) aggregation and interfacial instability. This study innovatively proposes a spatial confinement strategy by anchoring Cu NPs inside (Cuin/SBA-15) or outside (Cuout/SBA-15) the mesoporous channels of SBA-15, leveraging nanoscale confinement to optimize Cu–O–Si interfaces. The confined Cuin/SBA-15 catalyst demonstrated exceptional WGSR performance, achieving a reaction rate of 5.4 μmolCO·gcat−1·s−1, significantly surpassing conventional Cu/SBA-15 (3.1 μmolCO·gcat−1·s−1) and surface-loaded Cuout/SBA-15 (2.8 μmolCO·gcat−1·s−1), along with remarkable stability. This enhancement originates from the SBA-15 channels enabling the in situ formation of stable Cu–O–Si interfaces, which regulate the dynamic equilibrium between Cu0 (active for H2O dissociation) and Cu+ (critical for CO adsorption) species. In situ studies revealed their synergistic dynamic interconversion during WGSR, while domain confinement effects suppressed sintering by maintaining interfacial integrity. Kinetic and mechanistic analyses further identified the associative pathway, with HCOO* intermediate dissociation as the rate-determining step, facilitated by the stabilized Cu–O–Si interfaces. By resolving interfacial instability through confinement engineering, this work provides a paradigm for designing robust Cu-based catalysts, advancing both fundamental understanding and practical applications in WGSR and related heterogeneous catalysis.
研究领域:
催化
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材料科学
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化学工程
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纳米技术
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表面化学
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ACS Sustainable Chemistry & Engineering
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2021
·
IF 8.198
Xiangchen Kong,Chao Liu,Ming Lei,Feng Gong,Yue Han,Yuyang Fan,Ming Li,Rui Xiao
The fundamental understanding of the catalytic performance of copper-based catalysts for lignin hydroconversion is delayed compared with the empirical optimization of the catalyst preparation. Herein, we investigate the interplay between the lignin-abundant oxygen-containing functional groups and Cu active species via the catalytic β-O-4 lignin linkage hydrogenolysis. Catalyst performance data and elemental spectra characterizing the catalyst demonstrate the dominance of Cu0 in the catalysis. Remarkably, Cα–OH and Cα═O in the aliphatic chain play critical roles in this process, without which the linkage cannot be broken. These groups markedly accelerate the linkage cleavage by decreasing both the chemisorption energy between Cβ–O and Cu0 and the bond dissociation energy of the linkage. On the contrary, the methoxyl groups attached to the aromatic rings hinder the bond cleavage as a result of the steric effect. Such hindrance is significantly affected by the amount and position of the methoxyl groups. The results of this work highlight the importance of the unique structures of lignin in its reductive depolymerization catalyzed by copper-based catalysts, which appear to offer an opportunity for tailoring efficient copper-based catalysts for lignin hydrogenolysis.
研究领域:
化学工程
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催化
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可再生能源
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材料科学
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Shanguang Xu,Xin Han,Fan Zhang,Zhengyang Sun,Ruiying Chai,Fei Xu,Shanguo Du,Xiuling Jiao,Dairong Chen,Jie Zhang
The development of efficient catalysts for the selective hydrogenation of furfural (FAL) to furfuryl alcohol (FOL) is of great importance for sustainable chemical production. In this study, a highly efficient Cu/Al 2 O 3 catalyst was developed for the selective hydrogenation of FAL to FOL, achieving 100 % conversion and 100 % selectivity at 85 °C and 1.0 MPa H 2 with the optimal 7Cu/Al 2 O 3 -AIP catalyst, which was tailored by modulating the surface acidity of Al 2 O 3 and the distribution of Cu species. Evaluation of Cu-supported varying Al 2 O 3 catalysts revealed a near-linear correlation between the density of medium-strong acidic sites and catalytic activity, unequivocally demonstrating that medium-strong acidic sites on the alumina surface serve as the active sites for the reaction, which was further corroborated by competitive adsorption experiments involving pyridine and furfural. Furthermore, the density of Cu 0 sites was varied by adjusting the copper loading and conducting N 2 O selective oxidation experiments. Notably, a linear increase in catalytic activity was observed with the Cu 0 /(Cu 0 + Cu + ) ratio on the catalyst surface. Advanced characterization techniques, combined with experimental results, elucidated that the Cu 0 species act as the primary active sites for H 2 activation, while acidic sites are crucial for FAL adsorption, leading to the exceptional catalytic performance by the synergistic catalysis. This study underscores the synergistic effect between Cu 0 species and acidic sites, providing profound mechanistic insights into the FAL hydrogenation process and establishing a strategic foundation for the rational design of highly efficient Cu-based catalysts.
研究领域:
催化
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化学工程
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可持续化学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xiaoxiao Zheng,Jiaming Wang,Peipei Lei,Qihong Xue,Xian Kan,Jiangang Chen
An enhanced Cu + /Cu 0 catalytic structure via the electronic effect of K was fabricated; • The proper amount of K could regulate the ratio of Cu + /Cu 0 and promote Cu dispersion; • Both the enhanced Cu + /Cu 0 ratio and the smaller Cu size promote the generation of MG; • The increased basic sites by the K doping remarkably increase the ethers by-products; • The deactivation was caused by the boosted Cu + ratio and the coated active sites by K. In this work, the CuZr 2 catalysts with significantly enhanced Cu + /Cu 0 catalytic active structures via the electronic effect of K were synthesized by the means of citrate complexation and used for dimethyl oxalate (DMO) hydrogenation to methyl glycolate (MG). The CuZr 2 –1.0 K sample exhibited the most outstanding performance, achieving a DMO conversion of 93.4% and MG selectivity of 85.8%. And the role of K in Cu-based catalysts for DMO hydrogenation is universal. The reduction of the catalyst was inhibited after potassium addition, lowering the Cu 0 content, thus leading to a decrease in the H 2 adsorption capacity of the catalyst, and accordingly, its activity decreased. The results showed that the ratio of Cu + /Cu 0 increased after K doping, and the adsorption strength of the catalyst for H 2 was weakened, which inhibited the deep hydrogenation of DMO. Simultaneously, the smaller size of metallic Cu via the appropriate amount of K doping facilitated the desorption of MG. Therefore, the selectivity for the target product MG was remarkably improved. However, the basic sites on the catalyst surface could increase after K doping, which would lead to an increase in the ether by-products. As the reaction proceeded, the ability of the catalyst to adsorb and activate H 2 was diminished due to the significantly increased surface K content and Cu + ratio, leading to the deactivation of the K-doped catalyst. This study provides a potential pathway for alkali metals to regulate the electronic structure of Cu-based catalysts and apply them to the hydrogenation of DMO to MG. Download: Download high-res image (258KB) Download: Download full-size image
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