CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Pei-dong Wu,Lanyun Li,Hu Li,Zhen Fang
Sustainable upgrading of biomass to high-value chemicals is greatly dependent on catalytic C-C/C-O bond cleavage of high selectivity. Here, an oxidation-enhanced photoelectrochemical protocol was developed to be capable of breaking different types of C-C bonds for efficiently producing aromatic carboxylic acids (85.0–99.8% yields) from lignin. Ni local electronic state of the prepared F-Fe 2 O 3 -Co:NiO x H y with excellent durability could be modulated, and high-valence Ni(Ⅳ) reactive species played a key role in the oxidative C-C bond scission of various lignin models. In-situ characterization and control experiments indicated that photocatalytic radical and electrocatalytic interface facilitated C-H/O-H delocalization, contributing significantly to the enhanced oxidation process. In addition, quantum calculations elaborated that photo-excited holes and Ni(Ⅳ) are key reactive species for enhancive electrocatalytic cleavage of different C-C bonds in lignin to exclusively furnish aromatic carboxylic acids. This research provides a renewable funnel strategy for using solar energy to produce high-value mono-functional products from biomass.
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ACS Catalysis
·
2025
·
IF 13.1
Yang Chen,Diwen Zhou,Yongli Chang,Yunzhao Xu,Hongqiao Lin,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Lisheng Guo,Ting Qiu,Li Tan
The utilization of Rh-based catalysts in the direct production of ethanol from CO2 has been a subject of significant interest. However, to date, the precise active sites responsible for ethanol generation and the C–C coupling mechanism remain elusive. In this study, we present a Rh-based catalyst featuring nanoscale Rh–Fe alloy sites, which achieved an ethanol selectivity of 49.1% among all hydrocarbon and oxygenate products (CO excluded) under relatively mild reaction conditions (3.0 MPa, 200 °C, with a low metal loading of ≤1 wt %). The formation of ethanol proceeds via the HCOO* pathway with a CO insertion mechanism occurring at the alloy sites with a specific cluster size, where CH2* and CO* act as the crucial intermediates for C–C coupling. The electron interaction within the Rh–Fe alloy sites effectively reduces the energy barrier for the formation of the CH2CO* intermediate, thereby facilitating the production of ethanol. In contrast to the Rh–Fe alloy sites, the geminal-dicarbonyl binding configuration of CO* intermediates on Rh single sites favors the generation of byproducts such as methane and methanol, rather than ethanol. This research offers insights into the active sites and reaction mechanism of hydrogenation of CO2 to ethanol, thus enhancing the efficient utilization of Rh-based catalysts.
研究领域:
催化化学
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材料科学
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能源化学
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ACS Applied Energy Materials
·
2026
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IF 5.5
Tongxin Qu,Yongchun Zhao,Zhuo Xiong,Junying Zhang
Electrocatalytic CO2 reduction reaction (eCO2RR) offers a sustainable route for converting CO2 into value-added chemicals, contributing to carbon neutrality. While high selectivity toward C1 products has been achieved, the efficient production of multicarbon (C2+) compounds remains challenging due to the high energy barriers of C–C coupling. Copper-based catalysts are promising for C2+ generation owing to their unique *CO binding energy, yet they suffer from low selectivity and stability. Alloying copper (Cu) with other metals is an effective strategy for regulating intermediate adsorption and facilitating C–C coupling. In this study, an efficient CuGa solid solution alloy electrocatalyst for the eCO2RR was synthesized, employing only straightforward immersion drying and subsequent reduction annealing processes. At an applied potential of −1.19 V vs RHE, this catalyst exhibited a high Faradaic efficiency of 66.27% for C2+ products, significantly suppressing C1 pathways. It also demonstrated remarkable stability, maintaining structural and morphological integrity even after 12 h of electrolysis at a current density of 300 mA/cm2. Density functional theory calculation integrated with in situ characterization revealed that synergistic interaction between Cu and Ga enhances the adsorption of key intermediates (*COOH and *CO) and reduces the energy barrier of *CO dimerization. This work provides insights into the design of efficient and stable Cu-based electrocatalysts for C2+ production via an electrochemical method.
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JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
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2026
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IF 2.6
Liu Qidong,Wu Xiumei,Peng Yukang,Li Yunping,Yu Shu,Xiao Zian
SiZnOC gels were coated on C/C substrate by sol–gel, using methyltriethoxysilane (CH 3 Si(OCH 2 CH 3 ) 3 , MTES) and dimethyldiethoxysilane ((CH 3 ) 2 Si(OCH 2 CH 3 ) 2 , DMDES) as precursors, and zinc acetylacetonate (Zn(acac) 2 ) as the modifier. After pyrolysis under argon at 700 °C, SiZnOC ceramics were obtained. Microstructures of SiZnOC with different Zn/Si molar ratios were characterized by FTIR, XRD, SEM and XPS. Biocompatibilities of SiZnOC ceramics were measured by MTT, cell adhesion, antimicrobial activity of Escherichia coli and Staphylococcus aureus, DPPH free radical scavenging and reactive oxygen species (ROS) levels. Vitro bioactivities of materials were evaluated by the generation of bone-like hydroxyapatite (HA) in simulated body fluid (SBF). Results showed that antibacterial and antioxidant properties of SiZnOC enhanced with the content of Zn doping. When Zn:Si molar ratio of SiZnOC increased to 0.4, the inhibition zone diameters were the biggest of 6.7 mm and 5.4 mm for E. coli and S. aureus, respectively, and the scavenging rate was the highest of 88.9% for the DPPH free radicals. However, the level of intracellular reactive oxygen species (ROS) expression was promoted with the increase of Zn doping either. SiOC with Zn:Si molar ratio of 0.2 has the quickest speed of generation bone-like hydroxyapatite (HA) in SBF, on the balance of biocompatibility, bioactivity and antimicrobial performance, SiZnOC with Zn:Si molar ratio of 0.2 was the best for the moderate antimicrobial and antioxidant properties, and the qualified biocompatibility.
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ACS Catalysis
·
2026
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IF 13.6
Chaoxi Wang,Gong Zhang,Shuying Li,Xiaowei Du,Donglong Fu,Xiaoxia Chang,Zhi-Jian Zhao,Peng Zhang
Abstract Electrochemical CO reduction reaction (CORR) on copper is a prototypical platform for studying C–C coupling toward multicarbon (C2+) products, yet the fundamental factors governing this process remain under debate. Particularly, how electrolyte composition regulates interfacial proton transfer and thereby governs C–C coupling pathways is still unclear. This paper describes the role of alkali metal cations in controlling C–C coupling in CORR by restructuring interfacial water and modulating proton transfer dynamics on Cu electrodes. By varying cation identity (Li+, Na+, K+, Cs+) and concentration, we demonstrate that cations with intrinsic larger ionic radii in the electrolyte shift selectivity toward C2+ products. Combining differential electrochemical mass spectrometry (DEMS) analysis with in situ surface-enhanced Raman spectroscopy (SERS) and attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) investigations, it is revealed that alkali metal cations with large intrinsic radii have weak hydration shells that disrupt the interfacial hydrogen-bond (H-bond) network and increase the population of cation-coordinated water molecules at the interface, which may serve as more effective proton transfer channels toward surface intermediates. This reconstruction of interfacial water can accelerate *CO hydrogenation, thus promoting the C–C coupling for C2+ production. These findings identify interfacial water as an active regulator of interfacial proton transfer, thereby supporting a mechanistic link between electrolyte composition and C–C coupling pathways. This work emphasizes the importance of the interfacial microenvironment and molecular-level understanding of electrochemical reactions.
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Nature Nanotechnology
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2026
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IF 37.5
Han Xiao,Cui Peixin,Wu Geng,Cai Jinyan,Wang Chao,Sun Fanfei,Qiao Panzhe,Liu Xiaocheng,Zhuang Jiahao,Liu Huan,Su Fabing,Wang Gongming,Yan Wensheng,Qi Zeming,Lin Yue,Hong Xun,Li Yadong
Direct selective conversion of methane into high value-added chemical products has long attracted attention in both industry and academia. The production of C 2 oxygenates is especially challenging owing to the requirement for both C–H activation and C–C coupling. Here we report a boron nanosheet-supported Cu single atom with Cu–B 4 sites (Cu-SAs/B), which can effectively catalyse the conversion of methane to acetic acid with 97% selectivity and a high activity of 221.3 mmol g Cu −1 h −1 without the addition of CO. In situ X-ray absorption fine structure analysis reveals that Cu single atoms undergo reversible ‘switching’ to Cu 4 clusters under CH 4 oxidation conditions, enabling efficient C–H activation and C–C coupling. The switching behaviour is triggered by the presence of H 2 O 2 , and the coupling occurs between CH 3 * and CHO * intermediates formed on Cu single atoms and Cu clusters, respectively, as confirmed by in situ spectroscopic techniques. These findings provide a proof of concept for designing highly effective methane oxidation catalysts based on switchable nanocatalysts.
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Nature Communications
·
2026
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IF 18.1
Kong Xiangchen,Bie Leilei,Liu Chao,Wang Xing,Lan Wu,Bai Risheng,Xue Beichen,Li Tao,Zhang Huiyan,Barta Katalin,Xiao Rui
The depolymerization of condensed lignin—a byproduct of industrial pulping and biorefining—is crucial for sustainable biorefineries. However, it remains a formidable challenge due to the formation of recalcitrant C–C bonds during lignin isolation, restricting the reactivity and accessibility of the lignin macromolecule. Here, we demonstrate that a disordered crystalline mesoporous zeolite (Meso-Z) synergistically integrates strong acidity with enhanced mass transfer efficiency to process this bulk feedstock. Compared to conventional microporous zeolite, Meso-Z achieves 3.7–7.9 times higher yields (32.0–45.6 wt%) of aromatic monomers and dimers (MDs) from condensed lignin oligomers by C–C bond cleavage, thus enabling the total yields to exceed the theoretical maximum defined by C–O bond cleavage by 250–759%. Mechanistic studies reveal that this exceptional performance arises from Brønsted and Lewis acid-assisted hydrolysis and hydrogenolysis of C α –C aryl bonds, facilitated by the zeolite’s mesoporosity. Meso-Z also shows robust recyclability, maintaining stable catalytic activity over ten consecutive cycles. This work provides an efficient strategy for depolymerizing condensed lignin, paving the way for the valorization of industrial lignin streams.
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Nature Communications
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2026
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IF 18.1
Qi Ming-Yu,Tan Chang-Long,Tang Zi-Rong,Conte Marco,Sun Yugang,Xu Yi-Jun
Direct photocatalytic conversion of methanol into high-value multi-carbon chemicals through precisely controlled C − C coupling represents an extremely appealing but challenging goal. Herein, we demonstrate the efficient photoredox-driven dehydrocoupling of methanol into divergent synthesis of ethylene glycol and glycolaldehyde concomitantly with H 2 production by structural regulation of atomically dispersed Ni species. We showcase distinctly different reaction pathway for divergent C − C coupling of methanol over two types of atomically dispersed Ni cocatalyst-decorated SiO quantum dots, namely those with single Ni atoms (Ni 1 -SiO/SiO 2 ) and Ni clusters (Ni n -CdS/SiO 2 ). The Ni 1 -CdS/SiO 2 generates ethylene glycol with 90% selectivity by a radical homo-coupling pathway, whereas the Ni n -CdS/SiO 2 achieves 96% selectivity towards glycolaldehyde by a radical addition-elimination pathway. This work not only offers a fascinating nonpetroleum route for the divergent C–C coupling synthesis of ethylene glycol and glycolaldehyde but also underscores the broad vista of modulating non-selective radicals toward selective transformation of methanol into multi-carbon products.
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Nature Communications
·
2026
·Vol. 17
·期 1
·1383
·
IF 18.1
He Nan,Wang Bingsen,Sun Xisheng,Gao Qianwen,Xu Xinyi,Yang Yongfang,Dong Fagui,Miao Jie,Wang Haonan,Tang Dawei,Li Lin
Hydrovoltaic technologies face challenges of low conversion efficiency and narrow operational temperature ranges, limiting their practical applications in extreme environments. Here, we propose a molecular clustering strategy that leverages organic molecules to interact with organic salt anions, forming stable composite clusters. These clusters enhance water’s phase change energy barrier and thermal stability while mitigating electrostatic shielding effects, effectively overcoming ion transport bottlenecks across a wide temperature range. The hydrogel achieves an operational temperature range from −35 °C to 80 °C and increases power density by an order of magnitude compared to existing technologies. Furthermore, the hydrogel demonstrates exceptional thermal and mechanical stability, maintaining stretchability above 1000% and stable performance under harsh conditions such as freezing and high heat. These advancements enable hydrovoltaic systems to operate reliably in flexible electronics, environmental monitoring, and self-powered devices across extreme environments, providing sustainable energy solutions for diverse and demanding scenarios.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2016
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IF 1.34
Jun LI,Xin YANG,Zhe-an SU,Liang XUE,Ping ZHONG,Shuai-peng LI,Qi-zhong HUANG,Hong-wei LIU
C/C–ZrC–SiC composites with different ZrC–SiC contents were fabricated by precursor infiltration and pyrolysis. The effect of ceramic content on the microstructure and ablation resistance was investigated. Both the C/C–SiC and C/C–ZrC–SiC composites exhibited good ablation resistance under the plasma flame above 2300 °C. With the increase of ZrC content, a continuous oxide layer and a solid Zr–Si–O mesophase were formed during the ablation. And the structure of the formed oxides layer closely linked with the contents of ZrC–SiC ceramics. The solid ZrO 2 –ZrC and Zr–Si–O mesophase could increase the viscosity of SiO 2 moderately and improve the anti-scouring ability. The continuous SiO 2 –ZrO 2 –ZrC–SiC layer would serve as a thermal and oxygen barrier for preventing the substrate from further ablation. The C/C–ZrC–SiC composites with 27.2% ZrC and 7.56% SiC shows superior ablation resistance, and the mass and linear ablation rates are −3.51 mg/s and −1.88 μm/s, respectively.
研究领域:
材料科学
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陶瓷基复合材料
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高温材料
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烧蚀防护
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iScience
·
2023
·Vol. 26
·期 9
·107608-107608
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IF 5.8
Yujing Li,Huihui Luo,Shuo Wang,Lei Li,Guosong Li,Wen Dai
An unprecedented efficient protocol is developed for the oxidative cleavage of C≡C bonds in alkynes to produce structure-diverse esters using heterogeneous cobalt nanoparticles as catalyst with molecular oxygen as the oxidant. A diverse set of mono- and multisubstituted aromatic and aliphatic alkynes can be effectively cleaved and converted into the corresponding esters. Characterization analysis and control experiments indicate high surface area and pore volume, as well as nanostructured nitrogen-doped graphene-layer coated cobalt nanoparticles are possibly responsible for excellent catalytic activity. Mechanistic studies reveal that ketones derived from alkynes under oxidative conditions are formed as intermediates, which subsequently are converted to esters through a tandem sequential process. The catalyst can be recycled up to five times without significant loss of activity.
研究领域:
化学
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材料科学
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催化
·
有机合成
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
·
2022
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IF 3.322
Zhiming Wang,Yuedong He,Lijing Liao,Yuhao Zhang,Yucheng Zhao,Yibei Xiao,Xuefei Jiang,Fei Qiao
A glycosyl transferase , isolated from Angelica decursiva a medical herb rich in coumarin , shows C-glycosyl transferase activity by in vitro activity assay using 5,7-dihydroxycoumarin as substrate, producing a C-glycosylated product at position C′8 along with the main product at C′6 position. Catalytic promiscuity assay shows that Ad CGT also displays O- or C-glycosylation activity to other coumarins and flavonoids . When phloretin and 2,4,6-trihydroxyacetophenone were fed as substrates, Ad CGT catalyzed the formation of di-C-glycosides. Therefore, Ad CGT is a multifunctional glycosyltransferase with a broad substrate acceptability. This work highlights the potential of Ad CGT as a catalyst for glycosylation of coumarin and reveals a new regio-selective C-glycosyltransferase, providing a basis for exploring the mechanism of coumarin glycosylation.
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