ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Wei Jia,Hang Song,Dandan Wang,Chengfeng Zhou,Yuling Zhao,Yuandong Cui,Haoxi Ben,Xiaoli Yang
The sustainable conversion of cellulose to C2 alcohols (ethylene glycol and ethanol) represents a promising sustainable pathway to reduce reliance on fossil resources. However, achieving an effective balance between hydrolysis, C–C bond cleavage, and hydrogenation has remained a challenge. In this study, Pd/WOx catalysts with tunable Pd nanoparticle sizes (1.81–4.46 nm) were developed to investigate the structure–performance relationship. Catalytic evaluations revealed a volcano-type correlation between Pd particle size and C2 alcohol selectivity, with the 3Pd/WOx catalyst, featuring Pd nanoparticles averaging ∼3.0 nm, achieving a maximum selectivity of 78.5% under mild conditions (water solvent, 230 °C, 5 MPa H2, 4 h). Structural and chemical analyses revealed that smaller Pd clusters retained excess oxygen vacancies but lacked hydrogenation capacity, while larger Pd nanoparticles reduced accessible hydrogenation sites and acidity. Mechanistic studies showed that WOx oxygen vacancies promoted cellulose hydrolysis, Pd–O(H)–W sites facilitated glucose adsorption and C–C cleavage to glycolaldehyde, and adjacent Pd0 sites enabled efficient hydrogenation. This work highlights the critical role of Pd particle size in optimizing acid–hydrogenation synergy, providing a green and efficient strategy for biomass valorization without additives or toxic solvents.
研究领域:
催化
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纳米技术
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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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产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 61
·38486-38494
·
IF 3.361
Jun-Hao Zhou,Chen-Yue Yuan,Ya-Li Zheng,Hai-Jing Yin,Kun Yuan,Xiao-Chen Sun,Ya-Wen Zhang
Tandem catalysis, in which a CO2-to-C2 process is divided into a CO2-to-CO/*CO step and a CO/*CO-to-C2 step, is promising for enhancing the C2 product selectivity when using Cu-based electrochemical CO2 reduction catalysts. In this work, a nanoporous hollow Au/CuO–CuO tandem catalyst was used for catalyzing the eCO2RR, which exhibited a C2 product FE of 52.8% at −1.0 V vs. RHE and a C2 product partial current density of 78.77 mA cm−2 at −1.5 V vs. RHE. In addition, the C2 product FE stably remained at over 40% over a wide potential range, from −1.0 V to −1.5 V. This superior performance was attributed to good matching in terms of the optimal working potential and charge-transfer resistance between CO/*CO-production sites (Au/CuO) and CO/*CO-reduction sites (CuO). This site pair matching effect ensured sufficient supplies of CO/*CO and electrons at CuO sites at the working potentials, thus dramatically enhancing the formation rate of C2 products.
研究领域:
电化学
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催化
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材料科学
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能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Kai Zhu,Zihan Lin,Xinyi Bai,Fangfang Chang,Qing Zhang,Xiaolei Wang,Zhengyu Bai
Electrocatalytic reduction reaction of CO2 (CO2RR) into value-added multicarbon (C2+) products represents a sustainable strategy for mitigating greenhouse gas emissions and enhancing the production of high-value chemicals. Cu-based catalysts are optimal for the CO2RR, facilitating the generation of C2+ products such as ethanol, which have significant industrial applications. However, converting CO2 to C2+ products remains a great challenge, necessitating the simultaneous achievement of high current density, Faradaic efficiency (FE), and operational stability for industrial-scale implementation. Herein, we prepared Cu/Cu2O catalysts with diverse morphologies and the ratio of the Cu+/Cu interface, which was rectified by regulating the interactions between the active interface and the intermediate (*CO). The electrochemical analysis demonstrated that reconstructed Cu/Cu2O nanodendrites with dominant grain boundaries exhibited remarkable performance in generating C2+ products, achieving a Faradaic efficiency (FE) of 71.8%, including 49.7% FE of ethanol and a substantial partial current density of 390.0 mA cm–2 within the flow cell. In situ spectroscopy characterization and theoretical calculations revealed that the increased ethanol selectivity originated from the rectification of the Cu/Cu2O interface by the *CO intermediate, which accelerated H2O dissociation, reduced the free energy for *CO hydrogenation to *COH, and facilitated asymmetric *CO-*COH coupling to preferentially reduce CO2 to ethanol. This study provides profound insights into the C–C coupling pathways and sheds light on the rational design of ethanol-oriented electrocatalysts, contributing to sustainable chemical synthesis and energy utilization.
研究领域:
电催化
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能量转换
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材料科学
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环境化学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Junming Zhang,Xianchen Xu,Xin Guo,Na Liu,Xiongfeng Ma,Hongwei Ren,He Xiao,Man Zhao,Baoliang Lv,Jingxiao Tang,Tianjun Hu,Jianfeng Jia
Against the backdrop of global carbon neutrality target driving the transformation of energy structure, alcohol fuel cells (AFCs) show great application potential; However, the sluggish kinetics of their anodic alcohol oxidation reaction hinders the commercialization of AFCs. Metallene is a novel 2D material with potential application prospect in the field of electrocatalysis. In this paper, Pd 1 Mo 1 W trimetallene has been successfully produced by a one-pot wet-chemical method, which displays a unique two-dimensional curved ultrathin graphene structure. Mo and W atoms were doped into the lattice of Pd atoms to form a Pd 1 Mo 1 W ternary alloy, which resulted in the lattice spacing of Pd being enlarged to 0.229 nm and the d-band center of Pd being reduced by 1.10 eV. Therefore, Pd 1 Mo 1 W trimetallene demonstrated excellent electrocatalytic performance for the oxidation of ethanol and ethylene glycol in alkaline electrolyte. Especially for the ethanol oxidation reaction (EOR), Pd 1 Mo 1 W trimetallene exhibited excellent mass activity (7.55 A mg Pd −1 ) and intrinsic activity (13.5 mA cm −2 ), low apparent activation energy (41.8 kJ mol −1 ), and outstanding CO anti-poisoning ability. According to the nuclear magnetic resonance, in-situ fourier transform infrared reflection spectra, and density-functional theory calculations, it is revealed that the Pd 1 Mo 1 W trimetallene with high surface area formed by Mo-doping reduces the d-band center of the active site, facilitates the adsorption of OH species, and enhances the tolerance of CO-poisoned intermediate, so that EOR can be carried out through C1 and C2 pathways at a lower potential. Compared to the electrocatalytic EOR system, the photocurrent density of Pd 1 Mo 1 W trimetallene under xenon lamp irradiation increased by 1.73 times, which was mainly attributed to the electron resonance effect generated by Mo and W elements to promote the electron transfer to Pd. The excellent electrocatalytic ethanol and ethylene glycol performance of Pd 1 Mo 1 W demonstrates the great application potential of metallene for electrocatalysis.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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能量转换
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表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xueru Zhao,Jinlong Wu,Jiaxin Bai,Ting Zhang,Zhenli Lv,Maoxu Wang,Min Zhu,Jing Li,Feng Li
Cuprous oxide (Cu 2 O) is a promising material for photoelectrocatalytic CO 2 reduction (PEC-CO 2 RR); however, its widespread application is hindered by issues such as photocorrosion, structural instability, and low selectivity toward desirable products. In this work, a Cu 2 O-BiOBr nanohybrid catalyst with excellent visible light responsiveness are successfully developed using energy band structure matching and morphology modulation strategies. This heterostructure exhibits a three-dimensional bridge-like architecture composed of interwoven one-dimensional nanorods and two-dimensional nanosheets. Cu 2 O acts as a surface electron-rich active center, while BiOBr functions as both a co-catalyst and photogenerated electron storage, enabling efficient photoelectrocatalytic conversion of CO 2 under visible light irradiation. That is, the optimized Cu 2 O-BiOBr-2 catalyst achieves a C 2+ Faraday efficiency (FE) of 51% at −0.6 V vs. RHE, which is 2.55 times exceeding the pure Cu 2 O catalysts, The findings obtained from in-situ spectroscopic characterization reveal that the efficient transport channel of the constructed heterojunction enhances charge transfer efficiency at the catalyst interface and boosts redox capacity, improving both efficiency and stability of Cu 2 O in PEC-CO 2 RR. This work provides new insights for constructing novel heterojunctions.
研究领域:
材料科学
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光催化
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电化学
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可持续能源
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICO-BIOLOGICAL INTERACTIONS
·
2022
·
IF 5.168
Liangping Li,Wenqing Du,Hui Wang,Yufei Zhao,Zetian Huang,Yan Peng,Shulan Zeng,Guohai Zhang
p53 inactivation is a common feature in non-small cell lung cancer (NSCLC) resulting in NSCLC malignant transformation . Targeting serine 392 phosphorylation to restore p53 anticancer activity has proven to be an effective therapeutic strategy against NSCLC. A synthetic p53 activator, NA-17, has been developed that shows promise in preclinical models of NSCLC. However, NA-17 exhibits limited therapeutic efficacy in oncogene-driven tumors as well as relatively high toxicity to normal cells. It is possible that high efficiency and low toxicity p53 activators can be obtained by optimizing the leading molecule. Here, we performed high-throughput screening of compounds optimized based on NA-17 to identify new p53 activators. Two promising candidates named MX-C2 and MX-C3 were identified, both exhibited considerable therapeutic efficacy in oncogene-driven tumor models. Similar to NA-17, MX-C2/3 induced p53 activation via phosphorylating serine-392 without DNA damage. Both compounds showed broad antitumor activity in NSCLC cells and limited toxicity in normal cell lines. Moreover, MX-C2/3 suppressed tumor progression by arresting the cell cycle at G2/M phase, exhibiting a different mechanism of cell cycle arrest than NA-17. In addition, MX-C2/3 promoted the enrichment of p-p53 (s392) in mitochondria, leading to the conformational activation of Bak for cell apoptosis, which is consistent with NA-17. Finally, we demonstrated that MX-C2 significantly inhibited tumor growth without obvious systemic toxicity in oncogene-driven HCC-827 xenograft models. Collectively, we report two p53 activators with high-efficiency and low-toxicity that target p53 serine 392 phosphorylation for anticancer translational investigation.
研究领域:
肿瘤学
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分子生物学
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药理学
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癌症研究
✓ 已验证
DOI
PubMed
高影响因子
Science Advances
·
2022
·Vol. 8
·期 23
·
IF 14.957
Peixin Zhang,Yao Zhong,Yan Zhang,Zhenliang Zhu,Yuan Liu,Yun Su,Jingwen Chen,Shixia Chen,Zheling Zeng,Huabin Xing,Shuguang Deng,Jun Wang
One-step separation of C 2 H 4 from ternary C 2 H 2 /C 2 H 4 /C 2 H 6 hydrocarbon mixtures is of great significance in the industry but is challenging due to the similar sizes and physical properties of C 2 H 2 , C 2 H 4 , and C 2 H 6 . Here, we report an anion-pillared hybrid ultramicroporous material, CuTiF 6 -TPPY, that has the ability of selective recognition of C 2 H 4 over C 2 H 2 and C 2 H 6 . The 4,6-connected fsc framework of CuTiF 6 -TPPY exhibits semi–cage-like one-dimensional channels sustained by porphyrin rings and TiF 6 2− pillars, which demonstrates the noticeably enhanced adsorption of C 2 H 2 and C 2 H 6 over C 2 H 4 . Dynamic breakthrough experiments confirm the direct and facile high-purity C 2 H 4 (>99.9%) production from a ternary gas mixture of C 2 H 2 /C 2 H 6 /C 2 H 4 (1/9/90, v/v/v) under ambient conditions. Computational studies and in situ infrared reveal that the porphyrin moieties with large π-surfaces form multiple van der Waals interactions with C 2 H 6 ; meanwhile, the polar TiF 6 2− pillars form C–H•••F hydrogen bonding with C 2 H 2 . In contrast, the recognition sites for C 2 H 4 in the framework are less marked.
研究领域:
材料科学
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化学工程
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物理化学
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吸附分离
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多孔材料
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zong Li,Kaili Ni,Yifei Wang,Yuan Rui,Miaohui Wang,Haiping Lin,Peipei Huang,Qing Li
Achieving high activity and selectivity for multi-carbon (C 2+ ) products on copper-based catalysts at ampere-level current densities is important for advancing industrial electrochemical CO 2 reduction reaction (eCO 2 RR). However, oxidative copper species are prone to reduction to metallic copper at high reduction potentials, causing the decline of selectivity and stability for C 2+ products. Herein, we report that Cucurbit[6]uril (CB[6])-modified copper nanoparticles promote eCO 2 RR via stabilizing Cu + sites at ampere-level current densities. The Cu-CB[6]-3 catalyst exhibited the highest C 2+ productivity with a faradaic efficiency of 72.2 ± 1.0 % at a current density of 1.0 A cm −2 , and the corresponding potential was −1.2 V vs. RHE. Detailed systematical spectroscopic analyses revealed that the main reason for boosting the C–C coupling is that the strong coordination interaction and molecular-level confinement of CO 2 and reaction intermediates of CB[6] can not only stabilize Cu + at higher current densities, but also accelerate the reaction kinetics. Simultaneously, the hydrophobic inner cavity and hydrophilic outer surface of CB[6] molecules ensure the smooth progress of eCO 2 RR while suppressing the hydrogen evolution reaction, resulting in high C 2+ selectivity and long-term stability. This work provides an approach to design highly efficient catalysts for industrial eCO 2 RR.
研究领域:
催化
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电化学
·
材料科学
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化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 12
·6468
·
IF 4.9
Yuying Li,Wei Yan,Yu Qin,Liwei Zhang,Sheng Xiao
Chemotherapy resistance in cancer is an essential factor leading to high mortality rates. Tumor multidrug resistance arises as a result of the autophagy process. Our previous study found that compound 1-nitro-2 acyl anthraquinone-leucine (C2) exhibited excellent anti-colorectal cancer (CRC) activity involving autophagy and apoptosis-related proteins, whereas its underlying mechanism remains unclear. A notable aspect of this study is how C2 overcomes the multidrug susceptibility of HCT116/L-OHP, a colon cancer cell line that is resistant to both in vitro and in vivo oxaliplatin (trans-/-diaminocyclohexane oxalatoplatinum; L-OHP). In a xenograft tumor mouse model, we discovered that the mixture of C2 and L-OHP reversed the resistance of HCT116/L-OHP cells to L-OHP and inhibited tumor growth; furthermore, C2 down-regulated the gene expression levels ofP-gpandBCRPand decreasedP-gp’sdrug efflux activity. It is important to note that while C2 re-sensitized the HCT116/L-OHP cells to L-OHP for apoptosis, it also triggered a protective autophagic pathway. The expression levels of cleaved caspase-3 and Beclin 1 steadily rose. Expression of PI3K, phosphorylated AKT, and mTOR were decreased, while p53 increased. We demonstrated that the anthraquinone derivative C2 acts as an L-OHP sensitizer and reverses resistance to L-OHP in HCT116/L-OHP cells. It suggests that C2 can induce autophagy in HCT116/L-OHP cells by mediating p53 and the PI3K/AKT/mTOR signaling pathway.
研究领域:
肿瘤学
·
药理学
·
分子生物学
·
癌症研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Xiaoyan Liu,Pengyu Guo,Zhiwei Liu,Borong Zhang,Sijia Li,Xin Liu,Yunling Liu
Although the one-step separation of ethylene from C2 hydrocarbons remains a significant challenge, one-step C2 separation provides a revolutionary breakthrough in cost savings and efficient energy utilization. Recent advances in metal–organic frameworks (MOFs) for achieving one-step C2 separation have been widely recognized. In this work, for the first time, the potential relationship between the structure and properties of MOF materials previously used for one-step C2 separation was revealed from a mathematical statistical perspective. Additionally, the importance of N/O sites in enhancing the selectivity of C2H6/C2H4 separation is elucidated as a supplementary finding. Guided by the above findings, a pillar-layered MOF (JLU-MOF167) was synthesized using a mixed-ligand strategy. The unprecedented layer structure, composed of triazole units and multiple Cd units, provides an optimal thickness that creates a large number of N/O sites. Simultaneously, the tortuous channels between the pillars ensure sufficient interaction space between the molecules and the framework. The excellent structural design enables JLU-MOF167 to exhibit outstanding performance in both C2H2/C2H4 and C2H6/C2H4 separations as well as dynamic separation capabilities. Furthermore, theoretical calculations confirm the critical role of high-density N/O sites in facilitating one-step C2 separation.
研究领域:
材料科学
·
化学工程
·
分离技术
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无机化学
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Long Cheng,Rong Wang,Wenzhe Si,Yanxi Deng,Junhua Li,Yue Peng
Cu-based catalysts leveraging Cu+/Cu0 active sites have emerged as pivotal for synthesizing essential hydrocarbons and alcohols in electrochemical CO2 reduction, such as ethylene and ethanol (C2 products). However, the dynamic reduction of Cu+ to Cu0 during electroreduction leads to site instability, resulting in diminished efficiency for CO2 conversion to C2 products. Herein, we introduced Si into CuO by the selective dissolution method, engendering Cu–O–Si units to stabilize the Cu+/Cu0 sites. The catalyst manifested good activity in CO2 electroreduction with an elevated Faradaic efficiency for C2 products reaching 81.9% at −100 mA/cm2. After ten cycles of electrochemical testing, the Cu+/Cu0 sites and performance exhibited no signs of degradation. The Si incorporation significantly improved the hybridization of O 2p and Cu 3d orbitals, thereby reinforcing the Cu–O bonds and stabilizing the Cu+/Cu0 sites, which was critical in promoting C–C coupling via decreasing the energy barriers for *OCCO formation and enhancing C2 product selection. The active Cu+ cations with unsaturated coordination contributed to the reaction stabilization, thereby improving the preservation of Cu2O metastable state.
研究领域:
电化学
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催化
·
材料科学
·
能源转化
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Jingchi Zhang,Ze Hua,Ziqi Wu,Xinting Cao,Wen Yang,Ruiwen Shao,Yu Bai,Zhenhua Wang,Kening Sun
To satisfy the demands of modern society for high-energy–density sulfide-based all-solid-state lithium batteries (ASSLBs), Ni-rich cathode materials have gained much attention for their high capacity and energy density. However, their practical deployment is hindered by accelerated interface degradation and capacity decay originating from surface oxygen release and lattice oxygen activation during prolonged cycling. In this study, Ti x NbB (1− x ) C 2 was successfully coated on the surface of LiNi 0.94 Co 0.05 Mn 0.01 O 2 . Density functional theory (DFT) calculations first elucidate a “point-to-point” anchoring mechanism where each surface oxygen atom coordinates with single species (Ti/Nb/B) offered by Ti x NbB (1− x ) C 2 , which forms robust O–M bonds and sustain a stable interface structure. The electron energy loss spectroscopy (EELS) reveals the segregation of Ti/Nb toward subsurface layers during cycling, creating an optimized lattice oxygen coordination environment and suppressing oxygen activation. The dual oxygen stabilization mechanism dramatically improves the reversibility of phase transition and the structural stability of the Ni-rich cathode materials. Moreover, Ti x NbB (1− x ) C 2 as the protective layer decreases mechanical strain and suppresses the parasitic reactions. Consequently, the engineered cathode delivers 91% capacity retention after 1000 cycles at 0.3 C, suggesting excellent cycling stability. The research delivers a new design philosophy for the coating layer that can stabilize surface oxygen. Furthermore, the atomistic understanding of the structure–property relationship of the Ni-rich cathode materials provides valuable guidance for the future design of new cathode materials with superior structural stability in ASSLBs.
研究领域:
材料科学
·
电化学
·
储能
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电池技术
·
计算材料设计
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）