INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Zhengrong Xu,Yu Li,Quanxin Guo,Shuai Shao,Zhongxun Wei,Rui Liu
Electrochemical CO 2 reduction reaction (CO 2 RR) offers a promising route for converting greenhouse gases into valuable chemicals. Herein, we report the synthesis of Bi-doped indium (In Bi) nanoparticles supported on a carbon rod (In-Bi x @C). Bi incorporation tuned the electronic structure of In and enhanced the CO 2 RR activity. The optimized In-Bi 100 @C catalyst achieved a 92.7 % formate Faradaic efficiency at −1.2 V vs. RHE with a good stability This study provides insights into metal doping strategies for advancing CO 2 RR performance.
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ACS Catalysis
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2025
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IF 13.1
Xiaodong Wen,Qizhi Min,Xiaodong Liu,Gang Zhao,Junyao Wang,Qinshang Xu,Guoshuai Shi,Liming Zhang,Wenhua Zhang,Yude Su
Structural reconstruction─an uncontrollable process that compromises the stability of Cu-based catalysts in electrochemical CO2 reduction (CO2R)─presents a major scientific challenge that has yet to be overcome. In this work, we develop a well-controlled SiO2 encapsulation approach to stabilize Cu-based CO2R electrocatalysts against reconstruction. Using Cu nanowires (CuNWs) as a model platform, we demonstrate that SiO2 encapsulation can significantly suppress Cu reconstruction while retaining ∼95% of the initial CO2R performance over 24-h stability tests at −1.15 V vs reversible hydrogen electrode (VRHE). In contrast, unencapsulated CuNWs exhibit severe structural deterioration with attenuated CO2R activity under identical testing conditions. In situ Raman studies and density functional theory (DFT) calculations reveal that the antireconstruction effect results from the formation of a robust Cu–O–Si interface that can not only serve as a structural anchor but also contribute to strengthening the Cu–Cu bonding at the exposed Cu active sites during CO2R operation. These results decipher the stabilizing mechanism of SiO2 encapsulation, and provide key insights for designing durable Cu-based CO2R electrocatalysts toward practical applications.
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Molecular Catalysis
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2025
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IF 4.9
Bo Liu,Xin Zou,Zhenjiang Li,Ping Chen,Shengxin Chen,Xin Yuan,Yongzhu Hu,Yanqi Shi,Ziqi Liu,Kai Guo
The cycloaddition of CO 2 to epoxides (CCE) reaction is one of the few chemical processes viable commercially in the valorization of CO 2 . A bifunctional urea–phosphonium halide with both electrophilic and nucleophilic centers was proposed as an effective catalyst for CCE reactions here. The urea–phosphonium halides with different urea substituents and halide anions were simply synthesized and systematically evaluated in CCE reactions. It was found that the H-bond donicity of the urea N–Hs, the nucleophilicity of the halide anion, and the affinity between the urea and halide anions jointly affected the catalytic activity of the urea–phosphonium halide in CCE reactions. The H-bonding strength between the N–Hs and nucleophilic anions was disclosed via NMR titrations. The catalyst featuring a 3,5-bis(trifluoromethyl)phenyl-substituted urea structure and an iodide anion was selected as the optimal structure, which promoted the cycloaddition of styrene oxide with excellent conversion (92 %) and selectivity (99 %) in 6 h under mild conditions (1 mol% catalyst loading, 100 °C, 0.1 MPa CO 2 ). Furthermore, the bifunctional catalyst performed exceptional recyclability, exhibiting no discernible decline in catalytic activity over five consecutive reaction cycles. The structure−performance relationship of the urea–phosphonium halides and a wide range of substrates applicability provided valuable insights for the optimization of the existing catalysts or the further design of new effective organocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zhengang Zhou,Junjie Zheng,Lingyu Shao,Xiao Zhang,Chengjin Pan,Xiuqi Hu,Kai Feng,Hao Song,Shihan Zhang,Chenghang Zheng,Xiang Gao
Catalytic solvent regeneration has garnered significant attention due to its capacity to lower energy demands in industrial processes, promoting broader adoption of carbon capture systems. While progress has been made in catalyst engineering, creating efficient solid acid catalysts still encounters critical obstacles such as synthesizing mesoporous architectures with extensive surface areas and improving the spatial arrangement of active sites. Herein, this study developed a Ni/Fe@KIT-6 catalyst with ordered porosity and dual metal acid sites, leveraging the three-dimensional cubic pore structure of mesoporous silica to enhance liquid-solid mass transfer. The anchored Ni/Fe clusters synergistically enhanced proton transfer, reducing the activation energy of carbamate decomposition through optimized intermediate adsorption configurations. Catalytic testing revealed a 58.1 % enhancement in CO₂ desorption efficiency alongside a 41.2 % decrease in energy requirements relative to non-catalytic systems. The material maintained stable performance across multiple absorption-desorption cycles (efficiency decline <10 %), linked to the KIT-6 framework's retained structural stability and optimized metal-support bonding. Theoretical calculations revealed that the Ni/Fe dual sites lowered the CO 2 desorption reaction energy barrier, aligning with the enhanced CO₂ desorption efficiency. This synergistic interaction of dual metal acid sites within a high-surface-area architecture highlights viable pathways for scalable and energy-efficient CO₂ desorption, thereby advancing practical strategies for large-scale deployment of carbon capture technologies.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Shichen Zeng,Xu Liang,Mingang Zhao,Yanxiong Ren,Hanze Ma,Ziting Zhu,Yuhan Wang,Shaoyu Wang,Junyi Zhao,Guangzhaoyao Yang,Xuerui Wang,Fusheng Pan,Guangwei He,Zhongyi Jiang
Covalent organic frameworks (COF) are deemed as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, the size mismatch between the COF intrinsic pore and gas molecules becomes a grand challenge when using COF membrane for carbon capture. Herein, we propose a new type of polymer-functionalized COF laminar membranes through grafting CO 2 -phlic polyethyleneimine (PEI) polymer onto carboxylic acid COF (cCOF) laminar membranes. The cCOF nanosheets with high density of carboxyl groups are prepared via modified single phase solution method and then assembled to fabricate membranes. Further, the cCOF membranes are functionalized with PEI using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry. The introduction of abundant amino groups from PEI afford the affinity of membranes toward CO 2 . Meanwhile, the graft of the PEI polymers reduces the defects or pinholes on the membrane surface. As a result, the PEI functionalized cCOF membranes exhibit a high CO 2 permeance of 1004 GPU and a CO 2 /N 2 selectivity of 33.7, which reach the carbon capture target performance and show great prospect for treating real flue gas. Our approach of functionalizing cCOF membranes with tailored functionalities may inspire the design of molecule-selective COF membranes.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Deng Xianyu,Zhang Jianjun,Qi Kezhen,Liang Guijie,Xu Feiyan,Yu Jiaguo
Constructing S-scheme heterojunctions proves proficient in achieving the spatial separation of potent photogenerated charge carriers for their participation in photoreactions. Nonetheless, the restricted contact areas between two phases within S-scheme heterostructures lead to inefficient interfacial charge transport, resulting in low photocatalytic efficiency from a kinetic perspective. Here, In 2 O 3 /Nb 2 O 5 S-scheme heterojunctions are fabricated through a straightforward one-step electrospinning technique, enabling intimate contact between the two phases and thereby fostering ultrafast interfacial electron transfer (<10 ps), as analyzed via femtosecond transient absorption spectroscopy. As a result, powerful photo-electrons and holes accumulate in the Nb 2 O 5 conduction band and In 2 O 3 valence band, respectively, exhibiting extended long lifetimes and facilitating their involvement in subsequent photoreactions. Combined with the efficient chemisorption and activation of stable CO 2 on the Nb 2 O 5 , the resulting In 2 O 3 /Nb 2 O 5 hybrid nanofibers demonstrate improved photocatalytic performance for CO 2 conversion.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Hong Qian,Binxia Yuan,Yuhao Liu,Rui Zhu,Chengxi Zhang,Hexing Li
Photocatalytic CO2 reduction to renewable fuels presents a promising strategy to mitigate greenhouse effects, yet challenges persist in achieving high efficiency due to CO2’s thermodynamic stability and competitive H2O adsorption. Herein, we develop a superhydrophobic photochromic TiO2/Bi2Wo6 (TBW-2O) nanocomposite that synergistically enhances visible-light-driven CO2 reduction. Dynamic charge management via reversible W6+↔W5+ transitions not only suppresses charge recombination but also facilitates electron transfer for CO2 activation, as evidenced by in situ XPS and EPR. The superhydrophobic surface designed with sodium oleate (water contact angle >150°) selectively enriches CO2 at the active sites compared to H2O (ΔGCO2 = −2.88 eV vs ΔGH2O = −1.17 eV). Dual heterojunction effects (Type II + Z-scheme) between TiO2 and Bi2WO6 optimize light absorption and redox potentials. The optimized TBW-2O achieves exceptional CH4 and CO production rates of 48.09 and 37.40 μmol·g–1·h–1, respectively, representing 19.7- and 6.6-fold enhancements over pure TiO2. Notably, it attains an apparent quantum yield (AQY) of 0.35% (CH4) and 0.32% (CO) at 350 nm without sacrificial agents or noble metals. Combined experimental and theoretical analyses reveal that the W6+/W5+ redox cycle and hydrophobic interface collaboratively promote COOH/CHO intermediate formation, steering the reaction pathway toward CH4. This work provides a design blueprint for multifunctional photocatalysts integrating photochromism and surface wettability control.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Wang Kai,Hu Yanjun,Liu Xiufan,Li Jun,Liu Bin
Strain engineering offers an attractive strategy for improving intrinsic catalytic performance of a heterogeneous catalyst. Herein, we successfully create strain into layered indium sulfide (In 2 S 3 ) at atomic scale via introducing oxygen coordination and sulfur vacancy using a wet-chemistry method. The atomically strained In 2 S 3 exhibits greatly enhanced CO 2 photoreduction performance, achieving a CO 2 to CO conversion rate of 5.16 μmol g catalyst −1 h −1 under visible light illumination in ambient air. In-situ spectroscopic measurements together with theoretical calculations indicate that the atomically strained In 2 S 3 features lattice disordered defects on surface, which provides rich uncoordinated catalytic sites and induces structural distortion, resulting in modified band structure that promotes CO 2 adsorption/activation and boosts photogenerated charge carriers’ separation during CO 2 photoreduction. This work provides a new approach for the rational design of atomically strained photocatalysts for CO 2 reduction in ambient air.
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CHINESE JOURNAL OF CATALYSIS
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2025
·
IF 17.7
Xiao-Han Li,Bo-Wen Zhang,Wan-Feng Xiong,Ze Li,Xiao-Yu Xiang,Si-Ying Zhang,Duan-Hui Si,Hong-Fang Li,Rong Cao
Electrochemical reduction of carbon dioxide (CO 2 RR) is a promising approach to complete the carbon cycle and potentially convert CO 2 into valuable chemicals and fuels. Cu is unique among transition metals in its ability to catalyze the CO 2 RR and produce multi-carbon products. However, achieving high selectivity for C 2+ products is challenging for copper-based catalysts, as C–C coupling reactions proceed slowly. Herein, a surface modification strategy involving grafting long alkyl chains onto copper nanowires (Cu NWs) has been proposed to regulate the electronic structure of Cu surface, which facilitates *CO-*CO coupling in the CO 2 RR. The hydrophobicity of the catalysts increases greatly after the introduction of long alkyl chains, therefore the hydrogen evolution reaction (HER) has been inhibited effectively. Such surface modification approach proves to be highly efficient and universal, with the Faradaic efficiency (FE) of C 2 H 4 up to 53% for the optimized Cu–SH catalyst, representing a significant enhancement compared to the pristine Cu NWs (30%). In-situ characterizations and theoretical calculations demonstrate that the different terminal groups of the grafted octadecyl chains can effectively regulate the charge density of Cu NWs interface and change the adsorption configuration of *CO intermediate. The top-adsorbed *CO intermediates (*CO top ) on Cu–SH catalytic interface endow Cu–SH with the highest charge density, which effectively lowers the reaction energy barrier for *CO-*CO coupling, promoting the formation of the *OCCO intermediate, thereby enhancing the selectivity towards C 2 H 4 . This study provides a promising method for designing efficient Cu-based catalysts with high catalytic activity and selectivity towards C 2 H 4 .
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Nature Chemistry
·
2025
·
IF 20.2
Li Lei,Cui Chunhua
Electrocatalysis has long been viewed as an interfacial process, so the role of bulk water redox chemistry remains largely unexplored. Here we demonstrate that electrolyte-induced water redox radicals activate reactants in bulk solution for electrocatalysis at electrified interfaces. Using formate as a model electrolyte, we show that hydrogen-bond disruption in bulk water generates redox radicals, which oxidize formate to generate C 1 intermediates, as revealed by electron paramagnetic resonance, high-resolution mass spectrometry and Raman spectroscopy. Formate concentration-dependent hydrogen-bond restructuring drives the sequential generation of water-derived radicals and reactive intermediates, establishing bulk water as an active redox mediator rather than a passive solvent. In situ electrochemical studies demonstrate that these C 1 intermediates migrate to the Cu cathode surface, enabling C–C coupling via radical-mediated pathways. This work challenges the conventional view of electrocatalysis as solely an interfacial process and offers an alternative design principle for efficient electrochemical synthesis through tailored electrolyte engineering.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Bowen Xu,Chao Xu,Qiongqiong Jiang,Huajing Zhang,Fei Jin,Hailin Zhang
The isothermal thermochemical redox cycle is a promising route for solar-driven CO 2 splitting, as it enables stable heat input and simplifies reactor design. However, achieving high redox activity and long-term stability remains a challenge for oxygen carrier materials. In this study, spinel FeAl 2 O 4 foam ceramics were synthesized at three calcination temperatures for 1300 °C (FA-13), 1400 °C (FA-14), and 1500 °C (FA-15), to investigate the redox performance. X-ray diffraction patterns were tested and confirmed that FA-14 and FA-15 both exhibited a pure FeAl 2 O 4 phase, while FA-13 retained residual Al 2 O 3 . The structure characteristics and scanning electron microscopy analyses revealed that FA-14 exhibited optimal porosity (74.41 %) and uniform grain distribution. In contrast, FA-15 showed densification and reduced porosity (71.75 %), while FA-13 displayed structural defects and poor crystallinity. Isothermal CO 2 splitting tests at 1400 °C demonstrated that FA-14 achieved the highest CO yield of 206 μmol/g, outperforming CeO 2 , FA-13 and FA-15. Long-term cycling tests over 50-cycle redox test(>100 h) showed that FA-14 maintained stable CO and O 2 yields of 170 ± 10 μmol/g and 97 ± 5 μmol/g, respectively indicating excellent thermal stability under high-temperature operation condition. These results demonstrate that tuning the calcination temperature of FeAl 2 O 4 ceramics can optimize their redox performance by balancing crystallinity and porosity.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
·
IF 7.8
Pan Zhang,Zhongfa Zha,Jiawen Yang,Xinbo Wang,Jianwen Song,Shuming Du,Liwen Li,Kun Zhao,Dong Fu,Lemeng Wang,Jun Ke,Pengfei Qu
High energy consumption during CO₂ desorption remains a critical bottleneck limiting the industrial application of monoethanolamine (MEA)-based carbon capture technologies. To address this issue, a novel high-efficiency catalyst, the 1:4-Ti@D composite catalyst based on diatomite and TiO(OH) 2 surface modification, was developed. Catalytic performance was evaluated in 30 wt% MEA solution at 90 °C. Compared with non-catalytic processes, the 1:4-Ti@D catalyst enhanced total CO₂ desorption amount by 46.2 % and maximum desorption rate by 125.1 %, while reducing desorption energy consumption by 39.2 %. Notably, it maintained stable catalytic efficiency after 10 consecutive adsorption-desorption cycles, confirming its durability for industrial use. The physicochemical characteristics of the catalysts were comprehensively elucidated through various multi-dimensional characterization techniques. The experimental findings revealed that the synergistic effect of TiO(OH) 2 and diatomite substantially augmented the surface acid site density, while the optimized mesoporous structure facilitated efficient reactant transport, thereby underpinning the catalyst's exceptional performance. By the study of desorption mechanism, the stronger interaction between Ti and O of reactants can lead easier H 2 O and RNHCOO - absorption and activation. Moreover, an assessment of the catalyst's impact on thermal and oxidation degradation as well as the corrosion rate of MEA indicated minimal influence on amine degradation and corrosion processes. This work provides a new strategy for developing low-cost, high-stability clay-based catalysts and offers technical support for advancing energy-efficient industrial carbon capture systems.
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