DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 23
·9724-9731
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IF 3.5
Ying Peng,Shuo Chen,Zhengli Hu,Mengqi Yin,Lishun Pei,Qiaohua Wei,Zailai Xie
Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of −0.55 to −0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at −0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm−2 is achieved in a flow cell at −0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Yao Zhibo,Cheng Hao,Xu Yifei,Zhan Xinyu,Hong Song,Tan Xinyi,Wu Tai-Sing,Xiong Pei,Soo Yun-Liang,Li Molly Meng-Jung,Hao Leiduan,Xu Liang,Robertson Alex W.,Xu Bingjun,Yang Ming,Sun Zhenyu
The electrocatalytic reduction of CO 2 to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO 2 -to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO 2 to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO 2 . Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO 2 reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution.
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ACS Materials Letters
·
2024
·
IF 9.6
Cun Chen,Honggang Huang,Yao Chen,Zhe Zhang,Hui Fu,Hanjun Li,Wei-Hsiang Huang,Feili Lai,Nan Zhang,Tianxi Liu
Interface engineering has been widely explored due to its potential for regulating the intermediate adsorption, controlling mass/electron transfer, and preventing severe aggregation of catalysts. Hence, we have synthesized a series of Cu–In metallic aerogels (MAs) with a controlled ratio of Cu/Cu2In interfaces as efficient catalysts for electrochemical carbon dioxide reduction reaction (CO2RR). As a result, Cu–In MAs with the highest Cu/Cu2In interfaces abundance (Cu2In MAs) achieve the high Faradaic efficiency of CO up to 94.5% at −0.6 V vs reversible hydrogen electrode (RHE), outperforming Cu1In MAs, Cu3In MAs, Cu4In MAs, and Cu MAs. Furthermore, Cu2In MAs with the highest Cu/Cu2In interface abundance also exhibit excellent stability after continuous electrolysis for 10 h. Mechanism research indicates that the rich Cu/Cu2In interfaces in Cu2In MAs allow for moderate adsorption of CO2 and accelerate electronic transmission, which greatly reduce the energy barrier of the potential-limiting step, thus improving the CO2RR performance. This study indicates that interface engineering plays an important role in improving the CO2RR performance, providing a new strategy for preparing efficient CO2RR catalysts.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shujie Liang,Jiaxin Lv,Yishun Wang,Hong Deng
The development of efficient and stable single-atom catalysts (SACs) for CO 2 photoreduction is a persistent challenge. This study reports the successful preparation of SACs by incorporating isolated Ni atoms into carbon nanorods through a low-temperature calcination process using nickel bis(dimethylglyoximate) complexes. These Ni atoms, maintaining their original coordination environments, can facilitate charge separation, and enhance CO 2 adsorption and activation. The optimized catalyst exhibits a CO formation yield of 24.4 µmol with ∼96 % selectivity in high-purity CO 2 , outperforming both the precursor and pure carbon. Additionally, the Ni SACs showed strong catalytic selectivity in diluted CO 2 conditions, with selectivity rates of 82.57 %, 80.35 %, and 61 % at 0.1, 0.05, and 0.01 atm, respectively. This work provides critical insights for designing efficient visible light-responsive CO 2 photoreduction catalysts at the atomic level.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Hao Zheng,Guoliang Guo,Xiaoqiang Pei,Pengke Huang,Xiaoling Liu,Wenge Zheng
Elastomer foams with customized multimodal cellular structures have great application requirements in advanced fields, but a simple and practical way to realize it needs to be further studied. Herein, a strategy of presetting cells into elastomers before supercritical CO2 foaming was introduced to customize the cellular structures. Typically, taking olefin block copolymers (OBC, a thermoplastic elastomer with crystalline hard segments and rubbery soft segments) foams as an example, bimodal, sandwich, and gradient multimodal cellular structures were successfully prepared. The interaction between preset cells and newly nucleated cells during foaming had been systematically studied by controlling the morphology of preset cells and foaming conditions. It was found that the configuration of preset cells and the nucleation rate of small cells in OBC foams had a significant impact on their cellular structures. Specifically, the bimodal cellular structures can improve the expansion ratio and elasticity of OBC foams, and their rebounding ability could be improved by 14%, while their energy loss coefficient would be decreased by 17% (compared to homogeneous ones in this study). Furthermore, the feasibilities of this strategy in other elastomer foams (like POE, EPDM, and EVA foams) with bimodal cellular structures were also verified, which was expected to promote the development of high-performance elastomer foams.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yingnan Ma,Na Liu,Yulu Zhang,Zhen Xu,Juan Chen,Hong Wu,Jianqiang Meng
The gutter layer of thin film composite membranes (TFCMs) promotes the formation of ultrathin top layers. MOFs nanosheets gutter layer is an efficient strategy for building gas separation TFCMs while suffers from such an issue that gas molecules transport between interlayer thus making it difficult to fully utilize the excellent molecule sieving ability of MOFs. In this work, both MOFs nanosheets and continuous MOFs gutter layers were constructed to prepare TFCMs for CO 2 separation. The polyamide top layer with irregular structure was formed on MOFs gutter layer by interfacial polymerization. The physical and chemical properties as well as separation performance of different TFCMs were further compared. Benefitting from the denser structure and stronger hydrophobicity of continuous ZIF-8 gutter layer, the obtained top layer showed more regular structure with ultrathin thickness (≈30 nm). At the same time, due to the ZIF-8 gutter layer provided additional and stable CO 2 selectivity, the CO 2 permeance reached 588.2 GPU with the selectivity of CO 2 /N 2 and CO 2 /CH 4 of 49.8 and 52.3, which surpassed the 2008 Robeson upper bound. We believe that such a membrane design based on continuous MOFs gutter layers is a promising approach for high-performance gas separation membranes.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Zhaoxing Wu,Zhengxiong Wu,Yulai Zhao,Linxi Hou
The electrochemical reduction of CO2 to produce high-value multicarbon products represents a challenging yet highly desirable process, particularly due to the inefficient C–C coupling observed in current electrocatalysts. In this study, Cu2+ and Co2+ were introduced into ZIF-8 as precursors to synthesize a series of Co- and CuCo-doped carbon nanostructure materials with varying Co-to-Cu ratios. X-ray diffraction and X-ray photoelectron spectroscopy (XPS) analyses confirmed the successful doping of metal Co in the form of Co–Nx, while Cu was partly doped as nanoparticles attached to the carbon substrate surface and partly as single atoms forming Cu–Nx. Transmission electron microscopy and energy-dispersive X-ray spectroscopy analyses revealed uniform distribution of elemental Co and Cu on the carbon substrate, with Cu loaded as nanocluster on the surface. Linear sweep voltammetry tests indicated that Cu/CoCu-Nx-C composites exhibited enhanced reactivity toward CO2 reduction compared to other samples. At −0.19 V (vs RHE), the Faradaic efficiencies (FEs %) of C2H4, C2H6, CH4, CO, and H2 over Cu/CoCu-Nx-C were 29.7, 8.6, 20.2, 9.8, and 31.5%, respectively. The influence of Co and Cu doping modes on the selectivity of electrocatalytic reduction products was investigated. Results showed that Cu/CoCu-Nx-C exhibited a higher FE of C2 compared to Cu/Cu–Nx-C, with nearly 10 times higher C2 current density. Mechanistic insights from acid-etching experiments and XPS revealed a synergistic interaction between metallic Co and Cu, promoting the generation of multicarbon products. Co–Nx improved *CO coverage, facilitating subsequent C–C coupling on neighboring Cu–Nx. Additionally, CH4 production was attributed to the (111) crystalline facets in the Cu nanocluster and isolated Cu–Nx. Overall, this research provides an important understanding of the creation of straightforward and effective catalysts for the reduction of CO2. It holds considerable potential for the production of hydrocarbons using carbon dioxide.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Mingmin Jia,Xiong-Fei Zhang,Yicheng Zhou,Hengyang Mao,Yijiang Zhao,Jianfeng Yao
In this work, Amine-functionalized CNF/UiO-66 (CNF–NH 2 /UiO-66) composite membranes were fabricated by incorporating UiO-66 nanoparticles in the CNF–NH 2 matrix. The CO 2 -facilitated transfer channels can be constructed in the CNF–NH 2 /UiO-66 composite membrane. As a natural polymer material, CNF–NH 2 would absorb water and form a gel-like structure under humidification. The adsorbed water can convert CO 2 into bicarbonate ions (HCO 3 − ) through the catalysis of amino groups on CNF–NH 2 . Moreover, in CNF–NH 2 /UiO-66 composite membranes, HCO 3 − could quickly migrate to the permeate side promoted by the porous UiO-66, facilitating CO 2 transport. The optimum membrane gave a CO 2 permeability of 257.0 Barrer with a CO 2 /CH 4 ideal selectivity of 71.3.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Liu Hang,Liu Sixu,Liang Yaozhen,Sun Yifei,Xiong Haifeng
Palladium (Pd)-based catalysts are widely used for CO 2 hydrogenation reactions due to the capability to activate H 2 , which enhances the overall CO 2 conversion. However, most of the current Pd catalysts reported show high CO 2 conversion only at higher temperature, and the exploration of efficient catalyst enabling low temperature conversion (180–300 °C) is of importance. In this study, a series of Pd-B/ZnAl 2 O 4 catalysts were synthesized via in-situ doping, resulting in the Pd crystal transformation induced from crystal to amorphous. The catalytic hydrogenation activity of the amorphous Pd-B catalyst reaches its zenith at a Pd-B mole ratio of 1:2, accompanied by the superior catalysis stability in CO 2 hydrogenation. Various characterization techniques, including XRD, CO-DRIFTS, H 2 -TPR, XPS and TEM, were used to investigate the properties of the Pd-B/ZnAl 2 O 4 catalyst. The results showed that the Pd-B/ZnAl 2 O 4 catalyst exhibited higher dispersion and better CO 2 conversion efficiency compared to unmodified Pd catalyst. Additionally, the methanol space–time yields are nearly doubled when the B decoration is employed. At 280 °C, CO 2 conversion was improved and methanol selectivity remained at ~ 65%. This study provides valuable insights into the design and optimization of Pd-B based catalysts for CO 2 hydrogenation at low temperatures. Graphical Abstract
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yanqiu Wang,Ying Zhou,Xinxin Zhang,Mingrui Wang,Tangkang Liu,Jinxing Wei,Guanghui Zhang,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to higher alcohols (HA) is a promising route for high-value utilization of waste CO 2 , but developing active and stable catalysts remains a grand challenge. For this reaction, constructing multifunctional interfaces as active sites is required to fulfill controllable C-C coupling of alkyl and CO*/CH x O* species. Herein, we report a PdFe catalyst with abundant PdFe alloy-Fe 5 C 2 interfaces via a PdFe alloy induced FeO x carbidization process, which can achieve HA yield of 86.5 mg g cat −1 h −1 with 26.5% selectivity at 300 ºC, 5 MPa, and 6000 mL g cat −1 h −1 . The accelerated deactivation test unveils the PdFe catalyst exhibits better durability than the widely studied CuFe based catalysts against harsh conditions. Multiple in-situ characterization results unveil a synergetic mechanism for HA synthesis at the PdFe alloy-Fe 5 C 2 interfaces, where PdFe alloy is responsible for CO formation and non-dissociative activation, while Fe 5 C 2 phase promotes CO dissociation and chain propagation.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Manman Zhang,Liu Chen,Kaifang Wang,Ruitao Lin,Zeshen Xiao,Raphael Semiat,Xuezhong He
The development of materials has given rise to the study and design of poly(ionic liquid)s (PILs) for making CO2-selective membranes. The huge design space for the chemical structures of PILs provides great opportunities to further investigate the factors underlying gas permeability and selectivity. Herein, copolymerizing imidazolium-based ionic liquid (IL) monomers with two functionalized monomers of acrylamide (AM) and butyl acrylate (BA) based on free radical polymerization was conducted, and the effect of the chemical structures for PIL-based copolymers on their performances of derived membranes for CO2/N2 separation was evaluated. Nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectroscopy analysis confirmed the successful synthesis of copoly(ionic liquids) (co-PILs) with the designed chemical structures. The co-PIL-based composite membranes were fabricated by coating the copolymer solutions on the surface of a commercial polysulfone (PSF) membrane. It was found that the best composite membranes present significantly enhanced CO2 permeance (76 GPU) and CO2/N2 selectivity (53) by 262% and 61% compared to pure PSF membranes. The proposed coating method using co-PILs provides a facile solution to improve the CO2 separation membrane performance. Therefore, molecular engineering of the chemical structures for poly(ionic liquids) opens a venue to develop high-performance co-PIL-based membranes for potential CO2 capture from flue gases.
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Greenhouse Gases-Science and Technology
·
2024
·
IF 2.7
Lanxin Li,Zhibo Luo,Wei Zou,Shengke Liang,Hong Wang,Chen Zhang
Amine-functionalized porous polymers have been considered as a prominent chemical adsorption material for carbon capture and storage (CCS) process, because of their large adsorption capacity and high selectivity. By comparison, the low energy-consumption for desorption and high recyclability are the advantages of the physical adsorption approach. In this work, an amine-functionalized hierarchical porous polymer was prepared by HIPE (high internal phase emulsions) template and amine impregnation strategy, and applied as CO 2 adsorbent to realize chemical adsorption and physical adsorption simultaneously. First, a hierarchical porous matrix of poly(styrene-glycidyl methacrylate) was prepared by the HIPE method. The formed meso/micropores in the typical porous polymer matrix could attract CO 2 molecules, where the physical adsorption was achieved. Subsequently, PEI (polyethyleneimine) was impregnated into the porous polymer with abundant macropores, and the numerous of amino groups provided the reaction sites, where the chemical adsorption was achieved. As a result, an effective CO 2 adsorption material was obtained via controlling the porous structure by changing the volume fraction of dispersive phase, impregnation condition and amine loading. Aided by the chemical adsorption of amino groups, the CO 2 adsorption capacity of the obtained adsorbent reached 3.029 mmol/g. Moreover, the CO 2 adsorption thermodynamics confirmed the physicochemical synergistic adsorption, and then the Q st reduced to 31–42 kJ/mol and a good cyclic stability was obtained. As conclusion, the porous adsorbent showed a good industrial application prospect. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
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