Materials Today Communications
·
2023
·
IF 3.8
Mingchao Wang,Zhiji Zhou,Zilong Liang,Shaowen Du,Guoshuai Cai,Xiangjian Wang,Yunlei Zhou,Haijun Zhang
Hydromagnesite (HM) is a widely distributed primary natural carbonate mineral . To expand the application range of hydromagnesite and tap its fire-extinguishing potential, a new type of high-efficiency KHCO 3 @HM dry powder was prepared by coating potassium bicarbonate on the surface of hydromagnesite with a dip coating method. KHCO 3 @HM dry powder obtained a chemical inhibition effect through this method, and the fire extinguishing efficiency has been further improved. A series of tests were carried out to confirm the excellent physical and chemical inhibition effect of KHCO 3 @HM dry powder. Specific surface area tests showed that the specific surface area of KHCO 3 @HM dry powder (31.405 m 2 /g) was higher than NH 4 H 2 PO 4 dry powder (12.766 m 2 /g). Flowability tests showed that KHCO 3 @HM dry powder (0.04 g/s) achieved the same flowability as NH 4 H 2 PO 4 dry powder (0.04 g/s). Local oil basin fire experiments showed that the average fire extinguishing time of KHCO 3 @HM dry powder was shorter with less powder consumption. Under 0.2 MPa driving pressure, the fire extinguishing time of KHCO 3 @HM dry powder was 2.2 s faster than NH 4 H 2 PO 4 dry powder, and the dry powder consumption was 3.71 g less than NH 4 H 2 PO 4 dry powder. The cooling effect of KHCO 3 @HM dry powder (208 ℃) in 10 s was better than NH 4 H 2 PO 4 dry powder (157 ℃), and KHCO 3 @HM dry powder (399 ppm) showed a better smoke suppression effect than NH 4 H 2 PO 4 dry powder (545 ppm). The pyrolysis of KHCO 3 @HM dry powder reduced the fire temperature, diluted the oxygen concentration, and captured free radicals. The final pyrolysis products formed a thick oxide film to provide good heat insulation and asphyxiation effects. The excellent cooling, dilution, asphyxiation, and chemical inhibition mechanisms of KHCO 3 @HM dry powder were demonstrated, and finally achieved a comprehensive performance comparable to NH 4 H 2 PO 4 dry powder.
研究领域:
材料科学
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消防工程
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化学工程
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产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Jinsong Shi,Hongmin Cui,Jianguo Xu,Nanfu Yan,Shengyong You
Influences of porous carbon’s physicochemical properties on CO 2 adsorption vary with CO 2 pressure. The clarification of such complicated influences will undoubtedly be beneficial to the design and synthesis of carbonaceous adsorbents. To this end, in the current work we synthesized a series of N-doped hierarchically ordered micro-mesoporous carbons (NHOMCs). Ordered mesoporous polymer was synthesized with a solvent-free method using F127 as the soft template. After removing F127, the polymer was activated with KHCO 3 in the presence of urea at 700–800 °C. The obtained NHOMCs inherited the ordered structure of the polymer, and exhibited high surface area and nitrogen content. Synergistic effects of urea and KHCO 3 on nitrogen content and textural properties were discussed and revealed. At 25 °C, high CO 2 uptakes of 4.02 mmol/g (1 bar) and 15.42 mmol/g (20 bar) were achieved by the NHOMCs. We then systematically investigated the correlation between CO 2 uptake and physicochemical properties. The decisive factors of CO 2 uptakes at different pressures (1 bar, 5 bar, 10 bar, 20 bar) were analyzed. We believe the current work will provide helpful insights into the research of porous carbons for CO 2 adsorption.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Yunshuo Zhu,Lili Guan,Xiwen Song,Yarong Huang,Ming Li,Qingxian Zhang,Ruihua Guo
Strict control of carbon emissions is crucial for expediting the achievement of carbon neutrality. However, the current CO 2 RR electrocatalytic exhibits numerous shortcomings that impede the enhancement of catalytic activity. Issues such as lengthy catalyst preparation times, and high levels of precious metal content. Additionally, the aggregation of ultrafine nanoparticles contributes to a rapid deterioration in catalytic performance. Herein, a Joule-heating method is efficiently utilized to synthesize heterostructures nano-catalysts for CO 2 electroreduction on carbon cloth substrates. This method takes advantage of the thermoelectric coupling of the carbon cloth to achieve carbothermal reduction, while also regulating phase composition and introduction of oxygen vacancies. The Cu-CeO 2 /TiO 2 /CC catalyst synthesized in this method showed a current density in CO 2 of −32 mA·cm −2 at −1.0 V (vs. RHE). Notably, this catalyst demonstrated high CO selectivity and Faraday efficiency (FE CO ) of up to 82.5 % at a low potential of −0.3 V (vs. RHE). Optimal electrochemical performance is achieved at a power of 40 W. The ultra-fast temperature change process prevented the agglomeration of catalyst particles and facilitated the construction of a stable heterogeneous interface with a high oxygen vacancy concentration. In conclusion, this study presents a promising approach, particularly for the rapid preparation of low-cost, highly selective non-precious metal electrocatalysts.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Yueqi Feng,Jiaomei Xiao,Yiyi Qiu,Jianlin Huang
Precise control and understanding of surface changes in indium (In)-based catalysts during the electrocatalytic CO2 reduction reaction (CO2RR) process are challenging. This study presents a series of surface-reconstructed In2O3–Bi electrocatalysts, created by doping mesoporous In2O3 nanocubes with bismuth (Bi). This doping introduces abundant bimetallic In–Bi sites at the crystal–amorphous interfaces, enhancing the CO2-to-formate conversion selectivity. Bi atoms accelerate the surface reconstruction of In2O3, reduce the charge density around In atoms, and promote partial amorphization. In situ X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FT-IR) measurements and density functional theory (DFT) calculations show that the bimetallic In–Bi sites lower the energy barrier for the HCOOH* intermediate, enhance H2O dissociation, and inhibit the hydrogen evolution reaction (HER). The surface-reconstructed In1.8Bi0.2O3 electrocatalyst demonstrates a Faradaic efficiency (FE) of 92.6% and a partial current density of −28.5 mA·cm–2 and operates stably for 110 h in a H-type cell. In a flow cell, it achieves an FE of formate (FEformate) of 97.6% at −1.4 VRHE and maintains above 94% FEformate over a potential window of 800 mV (from −1.0 to −1.8 V vs RHE). This study offers an effective approach for designing high-performance electrocatalysts for the CO2RR based on surface reconstruction.
研究领域:
材料科学
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电催化
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2024
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IF 14.4
Yu-Qi Wang,Jiaju Fu,Yue Feng,Kaiyue Zhao,Lu Wang,Ji-Yuan Cai,Xiang Wang,Ting Chen,Fan Yang,Jin-Song Hu,Bingjun Xu,Dong Wang,Li-Jun Wan
The activity of the electrocatalytic CO2 reduction reaction (CO2RR) is substantially affected by alkali metal cations (AM+) in electrolytes, yet the underlying mechanism is still controversial. Here, we employed electrochemical scanning tunneling microscopy and in situ observed Au(111) surface roughening in AM+ electrolytes during cathodic polarization. The roughened surface is highly active for catalyzing the CO2RR due to the formation of surface low-coordinated Au atoms. The critical potential for surface roughening follows the order Cs+ > Rb+ > K+ > Na+ > Li+, and the surface proportion of roughened area decreases in the order of Cs+ > Rb+ > K+ > Na+ > Li+. Electrochemical CO2RR measurements demonstrate that the catalytic activity strongly correlates with the surface roughness. Furthermore, we found that AM+ is critical for surface roughening to occur. The results unveil the unrecognized effect of AM+ on the surface structural evolution and elucidate that the AM+-induced formation of surface high-activity sites contributes to the enhanced CO2RR in large AM+ electrolytes.
研究领域:
电化学
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催化
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表面科学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Liu Shikai,Li Yuheng,Wang Di,Xi Shibo,Xu Haoming,Wang Yulin,Li Xinzhe,Zang Wenjie,Liu Weidong,Su Mengyao,Yan Katherine,Nielander Adam C.,Wong Andrew B.,Lu Jiong,Jaramillo Thomas F.,Wang Lei,Canepa Pieremanuele,He Qian
The reconstruction of Cu catalysts during electrochemical reduction of CO 2 is a widely known but poorly understood phenomenon. Herein, we examine the structural evolution of Cu nanocubes under CO 2 reduction reaction and its relevant reaction conditions using identical location transmission electron microscopy, cyclic voltammetry, in situ X-ray absorption fine structure spectroscopy and ab initio molecular dynamics simulation. Our results suggest that Cu catalysts reconstruct via a hitherto unexplored yet critical pathway - alkali cation-induced cathodic corrosion, when the electrode potential is more negative than an onset value ( e.g ., −0.4 V RHE when using 0.1 M KHCO 3 ). Having alkali cations in the electrolyte is critical for such a process. Consequently, Cu catalysts will inevitably undergo surface reconstructions during a typical process of CO 2 reduction reaction, resulting in dynamic catalyst morphologies. While having these reconstructions does not necessarily preclude stable electrocatalytic reactions, they will indeed prohibit long-term selectivity and activity enhancement by controlling the morphology of Cu pre-catalysts. Alternatively, by operating Cu catalysts at less negative potentials in the CO electrochemical reduction, we show that Cu nanocubes can provide a much more stable selectivity advantage over spherical Cu nanoparticles.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Jianhao Li,Zhicheng Hu,Shuhuan Han,Dapeng Cao,Xiaofei Zeng,Jianfeng Chen
Electrocatalytic CO 2 reduction reaction (CO 2 RR) to multi-carbon product, especially for ethylene (C 2 H 4 ), provides a favorable pathway for carbon neutrality and renewable energy storage. However, the second-order C-C coupling reactions in CO 2 RR need always the high activation/driven energy in dynamics originating from the trace C 1 intermediate product. Herein, we synthesized the Ag-decorated Cu 2 O porous hollow core-shell catalyst named Ag@Cu 2 O where Ag nanoparticles uniformly distributed on inner the surface of the hollow Cu 2 O (H-Cu 2 O) via the sacrificial template method. Benefiting from the synergistic hollow structure and electron transfer from Cu and Ag to O, Ag@Cu 2 O catalyst delivers the excellent C 2 H 4 Faradaic Efficiency (FE) of 55 % ± 2 % at −1.0 V (vs. RHE), which is superior to the most reported catalysts. More importantly, in situ infrared spectroscopy and density functional theory (DFT) calculations reveal the introduction of Ag can decrease the activation energy required for *CO and C-C coupling.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Chen Xingbao,Lu Ruihu,Li Chengbo,Luo Wen,Yu Ruohan,Zhu Jiexin,Lv Lei,Dai Yuhang,Gong Shanhe,Zhou Yazhou,Xiong Weiwei,Wu Jiahao,Cai Hongwei,Wu Xinfei,Deng Zhaohui,Xing Boyu,Su Lin,Wang Feiyue,Chao Feiyang,Chen Wei,Xia Chuan,Wang Ziyun,Mai Liqiang
Bi-defect sites are highly effective for CO 2 reduction (CO 2 RR) to formic acid, yet most catalytic surfaces predominantly feature inert, non-defective Bi sites. To overcome this limitation, herein, tensile strain is introduced on wholescale non-defective Bi sites. Under rapid thermal shock, the Bi-based metal-organic framework (Bi-MOF-TS) shows weakened Bi–O bonds and produced tiny Bi clusters. During electrochemical reduction, these clusters create numerous continuous vacancies, inducing weak tensile strain over a large range of surrounding non-defective Bi sites. This strain enhances *OHCO intermediates adsorption and substantially lowers the reaction barrier. As a result, Bi-MOF-TS achieves a faradaic efficiency above 90% across 800 mV potential range, with an impressive formate partial current density of −995 ± 93 mA cm −2 . Notably, Bi-MOF-TS exhibits a high HCOOH faradaic efficiency of 96 ± 0.64% at 400 mA cm −2 in acidic electrolyte and a high single-pass carbon conversion efficiency (SPCE) of 62.0%. Additionally, a Zn-CO 2 battery with Bi-MOF-TS as the cathode demonstrates a peak power density of 21.4 mW cm −2 and maintains stability over 300 cycles.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 8
·1730-1739
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IF 5
Caitao Kang,Chenglong Ding,Yao Li,Yanming Li,Changli Li,Jingfu He
Electrochemical CO2 reduction (CO2R) in acidic electrolytes can effectively overcome the challenge of carbonate formation and poor carbon utilization efficiency of CO2R in alkaline and neutral electrolytes. The corresponding anodic reaction design in an acidic environment therefore becomes important to overcome the valueless products and high energy consumption of the oxygen evolution reaction (OER) that hinder the overall commercial value of CO2R systems. Herein, we designed an efficient coupling system of electrochemical CO2 reduction and chlorine oxidation in an acidic electrolyte to reduce CO2 loss and improve the sustainability of the reaction system. We modulated the local microenvironment to promote C–C coupling by combining the cation effect with the larger surface area CuO nanoparticle catalyst in an acidic electrolyte. As a result, this coupling system can achieve high C2H4 and Cl2 faradaic efficiencies (FEs) of 63% and 89% at 700 mA cm−2 simultaneously. The system is commercially promising as it stably produces valuable products at both the cathode and anode.
研究领域:
电化学
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能源转化
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催化科学
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产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2024
·Vol. 26
·期 48
·6844-6851
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IF 2.6
Yuyuan Chen,Yachang Huang,Xia Hu,Sijie Lin,De-Kun Ma
The exposed crystal facets of Cu have a profound effect on its electrocatalytic CO2 reduction reaction (CO2RR) activity and product selectivity. On the other hand, at present, most of the studies on Cu-based electrocatalysts for the CO2RR focus on the synthesis of C2+ products. There are only a few reports involving methanol (CH3OH) generation over Cu nanocrystals. Herein, CuO nanosheets (NSs) and nanorods (NRs) were synthesized through a controlled oxidation and dehydration route under mild reaction conditions, using Cu mesh as a Cu source and conductive substrate, respectively. The as-synthesized CuO NSs and NRs were further converted into Cu NSs and NRs through an in situ electrochemical reduction method, respectively. The experimental results showed that CH3OH could be efficiently produced over Cu NSs with abundant (111) crystal facets through the electrocatalytic CO2RR. The maximum CH3OH faradaic efficiency (FE) obtained on Cu NSs is 68% at a relatively low applied potential of −0.6 V vs. reversible hydrogen electrode (RHE), which is 1.6 times larger than that achieved on Cu NRs with primarily exposed (200) crystal facets (42%). The crystal facet-dependent electrocatalytic CO2RR activity toward CH3OH production was elucidated based on theoretical calculations combined with experimental results.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Pengxuan Wu,Wanbing Ma,Yuxin Ge,Jinbao Xu,Minglei Lu,Xia Li,Liang Ma,Song Bai,Tiejun Wang
A facile one-step method was developed to promote the carbon dioxide reduction reaction (CRR) activities to form the C2 products (C2H4 and C2H5OH) via the capping agent and organic solvent-free involvement of copper (Cu) on graphitic carbon nitride (GCN). By tuning the using amount of the Cu precursor, Cu-GCN-0.2 exhibited a total Faradaic efficiency (FE) of more than 86.69 ± 0.73% for the C1 species (CO, CH4, HCOOH) and C2 species (C2H5OH, C2H4) as the CRR products when the electrolysis was carried out at an overpotential of 0.7 V (vs RHE) even after 12 h electrocatalysis and at a ratio of about 1:1 for C2/C1. Further investigation confirms that the enhanced CRR activities can be ascribed to three aspects: Firstl’y, smartl’y regulation of the Cu involvement during the synthesis of GCN created the CRR active site, which enables more CO2 to be adsorbed and activated at a lower overpotential to participate in the C–C couple procedures. Secondly, the neglected HER active site was formed when Cu was involved, which enables the well-maintained proton generation and adsorption activities for the proton-coupled electron transfer procedures, leading to the promoted C2/C1 ratio. Thirdly, the decreased electronic resistance accelerates the electronic transfer speed, which enables a faster reaction rate and a promoted long-term durability performance. This research provides a facile method for the rational construction and preparation of the electrocatalyst toward large-scale utilization in sustainable conversion and application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhijian Chen,Zhenghui Ma,Guoli Fan,Feng Li
Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO2 reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO2 electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C2+ products at −1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm–2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH3CHO and *OC2H5 intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO2 electroreduction process.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）