ACS Catalysis
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2026
·
IF 13.6
Jingyi Wang,Zhan Gao,Shiwu Chen,Xuze Guan,Xinjie Luo,Wenlong Lan,Enqi Chen,Youxun Xu,Xin Ye,Jiaqi Yu,Chengzhi Guo,Yingying Fan,Hui Wang,Yang Lan
Direct selective conversion of methane under mild conditions remains a challenge. Photocatalytic nonoxidative coupling of methane (NOCM) offers a sustainable route to value-added hydrocarbons and hydrogen yet suffers from intrinsic trade-offs between activity, selectivity, and stability. Here, we report a charge-polarized Pt-Au nanoalloy on TiO2 that enables synergistic C2+ and H2 production in a continuous-flow photoreactor. The optimized Pt-Au/TiO2 exhibits C2+ and H2 yield rates of 22.3 ± 0.1 μmol h−1 (1115 ± 5 μmol g−1 h−1) and 21.2 ± 0.1 μmol h−1 (1060 ± 5 μmol g−1 h−1), respectively, with a C2+ selectivity of 99.0 ± 0.4% and stability over 210 h under light irradiation. The catalyst delivers an optimal balance of high product yields, near-quantitative C2+ selectivity, and stability under mild conditions, outperforming reported photocatalytic NOCM systems. In situ studies reveal that light-induced carriers partition at the bimetallic interface, where electrons preferentially localize on Pt sites and holes on Au sites, thereby establishing a Lewis acid-base-like, charge-polarized heterointerface. Au sites preferentially mediate *CH3 adsorption and selective C−C coupling, while Pt sites facilitate H2 evolution; the Pt-Au alloy synergy underpins C−C bond formation. This dual-site strategy harmonizes catalytic activity, selectivity, and stability, offering a generalizable approach for next-generation photocatalysts aimed at methane valorization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Zichen Song,Wenqian Wang,Jiantao Fu,Xiangbo Ma,Xiaolei Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
Ligand-directed inheritance creates asymmetric Cu–N/Cu–O motifs for CO 2 reduction. • Symmetry-breaking preserves highly active Cu δ+ interfaces under dynamic conditions. • Dual-mode *CO adsorption (atop/bridge) effectively bypasses C 2+ scaling laws. • Optimized sites lower C–C coupling barriers while poisoning hydrogen evolution. • Achieved 82.2% C 2+ FE at 0.9 A cm −2 with stable 50 h ampere-scale electrolysis. The electrochemical CO 2 reduction reaction (ECR) to multi-carbon (C 2+ ) chemicals is intrinsically hindered by the rigid scaling relations and geometric homogeneity of pristine copper surfaces, which enforce a singular atop-type *CO intermediate. Herein, we implement a ligand-directed motif inheritance strategy to synthesize nitrogen-doped CuO (N-CuO) nanoparticles, uniquely characterized by asymmetric Cu–N/Cu–O lattice motifs. Under severe cathodic polarization, these robust Cu–N bonds structurally modulate the metallic reconstruction, preserving local non-metal coordination to sustain a highly active, mixed-valence Cu δ+ species. Operando spectroscopic and theoretical analyses reveal that this local structural asymmetry disrupts adsorption homogeneity, explicitly driving the spatial co-adsorption of bridge- and atop-type *CO intermediates. This dual-mode configuration bypasses conventional kinetic bottlenecks to drastically accelerate C–C dimerization. Consequently, the N-CuO catalyst delivers a record-level C 2+ Faradaic efficiency of 82.2% at an industrially relevant current density of 0.9 A cm −2 , exhibiting exceptional structural and catalytic stability over 50 h of continuous flow-cell operation. This work establishes atomic-scale lattice asymmetry as a decisive design principle for stabilizing active Cu δ+ species and steering multi-carbon electrosynthesis at practical reaction rates. Download: Download high-res image (301KB) Download: Download full-size image A ligand-directed motif inheritance strategy is developed to precisely integrate asymmetric Cu–N/Cu–O motifs within the CuO lattice. This local structural asymmetry enforces the *CO atop /*CO bridge dual-mode co-adsorption, bypassing conventional scaling relations to lower the C–C coupling barrier while suppressing HER. The catalyst delivers a state-of-the-art C 2+ Faradaic efficiency of 82.2% at an industrially relevant 0.9 A cm −2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Cong Liu,Qing-shan Wang,Heng-fei Cui,Hao-wen Zhu,Ming-yang Liu,Rui-tang Guo
The highly selective generation of products in the photoelectrocatalytic (PEC) CO 2 reduction reaction is significantly hindered by the complex multi-electron transfer process. In this work, we designed and synthesized a Cu 2 O-Au@TiO 2 composite with a unique “core–shell–satellite” architecture via a facile wet-chemical approach. In this architecture, the Au nanocore strengthens visible-light harvesting through localized surface plasmon resonance (SPR) and injects hot electrons into the mesoporous TiO 2 shell, while the outer Cu 2 O selectively exposes highly active (111) facets and establishes low-mismatch interfaces with TiO 2 . This configuration promotes directional charge migration through virus-like synaptic channels, thereby accelerating multi-electron CO 2 reduction. The cooperative mechanism of SPR enhancement, crystallographic facet matching, and dynamic charge transfer enables efficient and selective conversion of CO 2 to C 2 H 4 . Under visible-light irradiation and applied potential, the optimized composite achieves a remarkable C 2 H 4 yield of 174 ± 3.2 μmol·cm −2 ·h −1 with a sustained current density exceeding 75 mA·cm −2 . These findings highlight a rational structural design that synergistically couples plasmonic excitation with interfacial charge management, establishing a promising paradigm for developing high-performance photoelectrocatalytic systems toward solar-driven CO 2 reduction.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Chen Qin,Tan Yao,Wang Xiqing,Wang Qiyou,Li Hongmei,Liu Kang,Fu Junwei,Chai Liyuan,Liu Min,Lin Zhang
Acidic CO 2 electroreduction to multi-carbon (C 2+ ) products using Cu-based catalyst has attracted considerable attention for CO 2 recycling due to high single-pass CO 2 utilization. However, its development is drastically limited by the poor stability, especially at high current density, caused by Cu dissolution/reconstruction during the reaction. Herein, we find the trace dissolved oxygen in the electrolyte accounts for the Cu dissolution/reconstruction and report an in-situ passivation strategy to prevent oxygen adsorption for inhibiting Cu dissolution/reconstruction for high stability CO 2 -to-C 2+ conversion. Theoretical and in situ spectroscopy demonstrate that aluminum citrate (AC) passivation layer decreases the adsorption of oxygen on Cu surface to effectively prevent the Cu oxidation, which is beneficial for the formation and adsorption of linearly bonded *CO toward C-C coupling. As the result, the Cu catalysts with AC layer achieve over 60% Faradaic efficiency C 2 H 4 and 38.7% energy efficiency to C 2+ for over 150 h stability at 500 mA cm −2 in strong acidic electrolyte.
研究领域:
电化学
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催化化学
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环境科学
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能源材料
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可持续化学
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二氧化碳利用
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界面科学
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ACS Catalysis
·
2024
·
IF 11.3
Chong Qi,Yifu Bi,Yaolin Wang,Hong Yu,Yuanyu Tian,Peijie Zong,Qinhua Zhang,Haonan Zhang,Mingqing Wang,Tao Xing,Mingbo Wu,Xin Tu,Wenting Wu
Nonthermal plasma (NTP) offers the potential for converting CH4 with CO2 into liquid products under mild conditions, but controlling liquid selectivity and manipulating intermediate species remain significant challenges. Here, we demonstrate the effectiveness of the Cu/UiO-66-NH2 catalyst in promising the conversion of CH4 and CO2 into oxygenates within a dielectric barrier discharge NTP reactor under ambient conditions. The 10% Cu/UiO-66-NH2 catalyst achieved an impressive 53.4% overall liquid selectivity, with C2+ oxygenates accounting for ∼60.8% of the total liquid products. In situ plasma-coupled Fourier-transform infrared spectroscopy (FTIR) suggests that Cu facilitates the cleavage of surface adsorbed COOH species (*COOH), generating *CO and enabling its migration to the surface of Cu particles. This surface-bound *CO then undergoes C–C coupling and hydrogenation, leading to ethanol production. Further analysis using CO diffuse reflection FTIR and 1H nuclear magnetic resonance spectroscopy indicates that in situ generated surface *CO is more effective than gas-phase CO (g) in promoting C–C coupling and C2+ liquid formation. This work provides valuable mechanistic insights into C–C coupling and C2+ liquid production during plasma-catalytic CO2 oxidation of CH4 under ambient conditions. These findings hold broader implications for the rational design of more efficient catalysts for this reaction, paving the way for advancements in sustainable fuel and chemical production.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Peng Yong,Xiong Hanting,Zhang Peixin,Zhao Zhiwei,Liu Xing,Tang Shihui,Liu Yuan,Zhu Zhenliang,Zhou Weizhen,Deng Zhenning,Liu Junhui,Zhong Yao,Wu Zeliang,Chen Jingwen,Zhou Zhenyu,Chen Shixia,Deng Shuguang,Wang Jun
Olefin/paraffin separations are among the most energy-intensive processes in the petrochemical industry, with ethylene being the most widely consumed chemical feedstock. Adsorptive separation utilizing molecular sieving adsorbents can optimize energy efficiency, whereas the size-exclusive mechanism alone cannot achieve multiple olefin/paraffin sieving in a single adsorbent. Herein, an unprecedented sieving adsorbent, BFFOUR-Cu-dpds (BFFOUR = BF 4 - , dpds = 4,4’-bipyridinedisulfide), is reported for simultaneous sieving of C 2 -C 4 olefins from their corresponding paraffins. The interlayer spaces can be selectively opened through stronger guest-host interactions induced by unsaturated C = C bonds in olefins, as opposed to saturated paraffins. In equimolar six-component breakthrough experiments (C 2 H 4 /C 2 H 6 /C 3 H 6 /C 3 H 8 /n-C 4 H 8 /n-C 4 H 10 ), BFFOUR-Cu-dpds can simultaneously divide olefins from paraffins in the first column, while high-purity ethylene ( > 99.99%) can be directly obtained through the subsequent column using granular porous carbons. Moreover, gas-loaded single-crystal analysis, in-situ infrared spectroscopy measurements, and computational simulations demonstrate the accommodation patterns, interaction bonds, and energy pathways for olefin/paraffin separations.
研究领域:
化学工程
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材料科学
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石油化学
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FOOD CHEMISTRY
·
2018
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IF 4.946
Jiangkun Dai,Wenjia Dan,Nian Li,Ruixue Wang,Yao Zhang,Nannan Li,Ruizhi Wang,Junru Wang
Thirty-one canthin-6-one analogues, mainly including C 2 or C 5 or D ring modified canthin-6-ones, were designed and synthesized in order to study their antibacterial activity and structure-activity relationships. The analogue 28 with the highest bioactivity had a peak minimum inhibitory concentration of 4 μg/ml and showed low cytotoxicity against L02 cells and good “drug-like” properties. The antibacterial effect of 28 was characterized further by scanning electron microscopy, cytoplasmic β -galactosidase leakage assay, molecular docking evaluation, UV–visible analysis and isothermal titration calorimetry (ITC) measurement. The results showed that 28 may exert its bactericidal effect by damaging bacterial cell membranes and disrupting the function of DNA topoisomerases, both of which could lead to rapid cell death.
研究领域:
药理学
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有机化学
·
微生物学
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JOURNAL OF APPLIED TOXICOLOGY
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2021
·Vol. 41
·期 12
·2011-2020
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IF 3.446
Yuanyuan Zhang,Bingke Ma,Shuangshuang Hao,Jiaqi Wang,Ruichen Zhang,Muhammad Ishfaq,Chenxi Shi,Liang Yuan,Rui Li,Changwen Li,Fangping Liu
Drug-induced liver injury (DILI) is a serious and frequently occurring issue in drug development. The c-Jun N-terminal kinase (JNK) signaling pathway plays an important role in many diseases; hepatocyte nuclear factor-1α (HNF-1α) and glutathione S-transferase A1 (GSTA1) are important in regulating liver-specific genes expressions and affecting drug metabolism. Oltipraz is used to treat liver cirrhosis by improving liver function, and C2-ceramide is a pro-apoptotic lipid that regulates multiple signaling pathways. In this study, we investigated the function of the JNK signaling pathway with HNF-1α and GSTA1 in a cellular model of DILI and whether oltipraz and C2-ceramide exert effects via the JNK pathway. The results showed that inhibiting JNK could ameliorate APAP-induced hepatocyte injury, reduced oxidative stress, suppressed JNK and c-Jun activation, and hepatocyte apoptosis. Meanwhile, the mRNA and protein expressions of HNF-1α and GSTA1 were increased significantly compared to control conditions. The effect of oltipraz (8 μmol/L) was similar to a JNK inhibitor and significantly increased HNF-1α/GSTA1 expression, but oltipraz combined with JNK inhibitor did not show a synergistic effect. Although C2-ceramide (8 μmol/L) aggravated hepatocyte injury and apoptosis, exacerbated oxidative stress, increased phosphorylation of JNK and c-Jun, and markedly decreased HNF-1α/GSTA1 expression, C2-ceramide combined with JNK inhibitor could partially alleviate these alterations. These results demonstrated that the JNK signaling pathway with HNF-1α/GSTA1 are involved in the process of DILI. Inhibiting JNK up-regulated HNF-1α and GSTA1 expressions which could attenuate hepatocyte injury. Oltipraz and C2-ceramide might affect the expression of HNF-1α/GSTA1 though JNK signaling.
研究领域:
药理学
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肝脏病学
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分子生物学
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CELL AND TISSUE RESEARCH
·
2022
·Vol. 390
·期 2
·293-313
·
IF 4.051
Li Zhen-Fang,Hao Shuang-Li,Wang Lan-Min,Qi Hong-Yu,Wang Jia-Ming,Tan Fu-Qing,Yang Wan-Xi
Spermatogenesis is a finely regulated process of germ cell proliferation and differentiation that leads to the production of sperm in seminiferous tubules. Although the mammalian target of rapamycin (mTOR) signaling pathway is crucial for spermatogenesis in mammals, its functions and molecular mechanisms in spermatogenesis remain largely unknown in nonmammalian species, particularly in Crustacea. In this study, we first identified es-Raptor (the core component of mTOR complex 1) and es-Rictor (the core component of mTOR complex 2) from the testis of Eriocheir sinensis . Dynamic localization of es-Raptor and es-Rictor implied that these proteins were indispensable for the spermatogenesis of E. sinensis. Furthermore, es-Raptor and es-Rictor knockdown results showed that the mature sperm failed to be released, causing almost empty lumens in the testis. We investigated the reasons for these effects and found that the actin-based cytoskeleton was disrupted in the knockdown groups. In addition, the integrity of the testis barrier (similar to the blood-testis barrier in mammals) was impaired and affected the expression of cell junction proteins. Further study revealed that es-Raptor and es-Rictor may regulate spermatogenesis via both mTORC1- and mTORC2-dependent mechanisms that involve es-rpS6 and es-Akt/es-PKC, respectively. Moreover, to explore the testis barrier in E. sinensis , we established a cadmium chloride (CdCl 2 )–induced testis barrier damage model as a positive control. Morphological and immunofluorescence results were similar to those of the es-Raptor and es-Rictor knockdown groups. Altogether, es-Raptor and es-Rictor were important for spermatogenesis through maintenance of the actin filament network and cell junctions in E. sinensis.
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Catalysts
·
2021
·Vol. 11
·期 5
·535
·
IF 4.146
Shuaikang Zhu,Xiaona Ren,Xiaoxue Li,Xiaopo Niu,Miao Wang,Shuang Xu,Zheyuan Wang,Yunxi Han,Qingfa Wang
The copper-based catalyst is considered to be the only catalyst for electrochemical carbon dioxide reduction to produce a variety of hydrocarbons, but its low selectivity and low current density to C2products restrict its development. Herein, a core-shell xZnO@yCu2O catalysts for electrochemical CO2reduction was fabricated via a two-step route. The high selectivity of C2products of 49.8% on ZnO@4Cu2O (ethylene 33.5%, ethanol 16.3%) with an excellent total current density of 140.1 mA cm−2was achieved over this core-shell structure catalyst in a flow cell, in which the C2selectivity was twice that of Cu2O. The high electrochemical activity for ECR to C2products was attributed to the synergetic effects of the ZnO core and Cu2O shell, which not only enhanced the selectivity of the coordinating electron, improved the HER overpotential, and fastened the electron transfer, but also promoted the multielectron involved kinetics for ethylene and ethanol production. This work provides some new insights into the design of highly efficient Cu-based electrocatalysts for enhancing the selectivity of electrochemical CO2reduction to produce high-value C2products.Keywords:CO2electrochemical reduction;core-shell structure;ZnO@Cu2O;synergy effect;C2products selectivity
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Y.L. Zhao,G.G. Li,H.M. Hou,J.C. Shi,S.N. Luo
We investigate atomic and molecular emission of laser-ablated nitromethane in an Ar or N 2 buffer gas, with fs laser-induced breakdown spectroscopy. The electronic bands of CN, C 2 , and NH molecules and the atomic transition lines of C I, N I, and H α are identified. The time series of the emissions are obtained, and the formation mechanisms of CN and C 2 are deduced. The CN violet system, the B 2 Σ + -X 2 Σ + (0-0) band, is chosen to extract plasma temperature from the experimental spectra.
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ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 27
·12026-12036
·
IF 7.6
Zhong Haojia,Liu Hongchen,Yang Fan,Sun Xinyang,Gao Fuming,Zhang Xiaona,Wei Kexin,Wang Kuobo,Li Shijia,Li Zhenxing,Wang Chunxia,Li Yongfeng
Copper-based electrocatalysts demonstrate significant potential for electrochemical CO 2 reduction toward value-added chemicals. However, achieving selective synthesis of multi-carbon (C 2+ ) products on copper-based catalysts remains a substantial challenge. In this study, a Cu 2 O electrocatalyst (Mg 0.1 -Cu 2 O-SC) doped with magnesium (Mg) and surface-modified by sodium citrate (SC) was successfully synthesized via a simple wet chemical reduction method. The Mg 0.1 -Cu 2 O-SC achieves a Faradaic efficiency (FE) of 77.8% and a partial current density of 357.9 mA cm −2 for C 2+ products, which is 1.35 times higher than the FE of unmodified Cu 2 O. Mg 0.1 -Cu 2 O achieves an enhancement in the FE for CO, demonstrating that the Lewis-acidic Mg weakens the bond strength of Cu−*CO and enhances the local concentration of *CO by attracting electrons from Cu. In situ spectroscopic analysis reveals that the surface modification of SC facilitates the *CO to *CHO hydrogenation, which shifts the C−C coupling to a more favorable *CO−*CHO route with a lower-energy barrier and consequently improves the FE for C 2+ products. Theoretical calculations indicate that the electron-withdrawing effect of Mg induces a downward shift in the copper d-band center. Energy barrier analyses reveal that SC effectively lowers the energy barriers for both the water dissociation reaction and the *CO−*CHO coupling reaction. This work confirms that Mg effectively modulates the adsorption behavior of key intermediates and synergistically optimizes the reaction pathway in concert with SC.
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