PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 16
·9188-9195
·
IF 3.945
Xifeng Luo,Ran Jiang,Ziang Ma,Tiantian Yang,Hui Liu,Hui Deng,Wenhong Wu,Cunku Dong,Xi-Wen Du
The work function can serve as a characteristic quantity to evaluate the catalytic activity due to its relationship with the surface structure of a material. However, what factors determine the influence of the work function on the electrochemical performance are still unclear. Herein, we elucidate the effect of the work function of Ag on the electrochemical reduction of CO2 to CO by controlling the ratio of exposed crystalline planes. To this end, the exposed surface of Ag powder was regulated by high-energy ball milling and its influence on CO2 reduction was investigated. The surface structure with more Ag(110) surface achieves higher activity and selectivity for CO production, resulting from the lower work function of Ag(110), which dramatically enhances the electron tunnelling probability during CO2 electroreduction. We found that a higher ratio of Ag(110) to Ag(100) leads to a lower work function and thus better electrochemical activity and selectivity. This study demonstrates a promising strategy to enhance the electrochemical performance of metal catalysts through tuning their work functions via regulating exposed crystalline planes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Ming Tang,Jia-Yi Du,Jin-Ling Ma,Xiao-Dong Wang,Xiong Zhang,Qin-Yin Shen,Fei-Peng Wang,Yu Wang
As the high energy-density energy storage and greenhouse gas capture device, Na-CO 2 battery development is impeded by the sluggish CO 2 reduction and difficult decomposition of insulating discharge products on the cathode. Here, the cobalt (Co)-decorated carbon nanofibers accompanying with slight Co oxidation were used as the self-standing cathode for Na-CO 2 battery. It greatly reduces the discharge overpotential by 500 mV and charge overpotential by 210 mV, delivers a 12 times higher discharge capacity and runs nearly 4 times cycle life than its counterpart. Experiment combined with theory calculation demonstrates that the evenly dispersive, abundant and stable active sites (Co-CoO) with an equal CO 2 adsorption-desorption capability is the key to improving cell performance. This work reveals the importance of catalysts/cathodes and provides a direction to design highly efficient catalysts/cathodes for alkali metal-CO 2 batteries.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Sustainability
·
2022
·
IF 7.244
R. Zeng,G. Jin,D. He,L. Zhang,D. Chen,Y. Zhang,L. Zhu,Y. Mei,W. Wu,Y. Luo
Utilizing propane and CO 2 as coreactants to produce syngas (CO/H 2 ) via dry reforming shows several advantages over direct propane dehydrogenation and traditional methane dry reforming . It is of great importance to establish high-efficiency catalytic systems that can break C–C bonds and activate CO 2 simultaneously. Herein, acidic H 2 O 2 was applied to etch LaCoO 3 . Surprisingly, highly dispersed Co 3 O 4 at the edges of support along with high oxygen vacancies were obtained from acidic H 2 O 2 treatment. Furthermore, the treated LaCoO 3 catalyst facilitated the generated intermediates of formate to convert into the desired products. The results showed that acidic H 2 O 2 treated LaCoO 3 catalyst can reach 18% for propane conversion and 35% for CO 2 conversion at 550 °C, showing high catalytic activity . Consequently, the present work provides some ideas for the synthesis of efficient LaCoO 3 catalysts for dry reforming of propane.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Jiuli Han,Haiyan Jiang,Shaojuan Zeng,Yinge Bai,Xiangping Zhang,Lu Bai
Mixed matrix membranes (MMMs) have drawn much interest in CO 2 separation due to their excellent separation performance, mechanical property, and desirable processability. However, obtaining highly compatible MMMs is a great challenge and is vital to avoid the loss of the separation selectivity of the MMMs. In this work, superbase ionic liquid (1,8-diazabicyclo[5,4,0]undec-7-ene imidazole ([HDBU][Im])) was used as a wetting agent to increase the interfacial compatibility between ZIF-67 and PIM-1, hence improving the membrane gas separation. [HDBU][Im] embeding into the MMMs could efficiently enhance the compatibility and diminish the interfacial voids. Furthermore, incorporating 5 wt% [HDBU][Im]@ZIF-67 nanocomposite into the PIM-1 matrix improves the gas permeability and CO 2 selectivity. The separation performances under the different temperatures were also conducted and showed that reducing temperature slightly decreases the gas permeability but significantly increases the CO 2 /CH 4 selectivity via enhancing the CO 2 solubility. The permeation active energies, diffusivities and solubilities were obtained to explain the gas permeate mechanism.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Xiaochun Hu,Yuqing Luo,Xianyue Wu,Jiabin Niu,Mingwu Tan,Zhiqiang Sun,Wen Liu
Heteroatom-doped microporous carbon nanosheets (HMCNs) are used in a wide range of applications, including gas adsorption, energy storage, and catalysis. Here, we demonstrate a solvent-free, template-free, one-pot polycondensation approach for the synthesis of HMCNs using melamine (MEL) and pentaerythritol (PER) as precursors. By varying the ratio of MEL to PER and the pyrolysis temperature, the doping amount, surface area and porosity of the HMCNs can be controlled. When used for CO 2 capture, the HMCN synthesized by the pyrolysis of a 3:2 mixture of MEL and PER at 900 °C (3/2-HMCNs-900) affords a CO 2 uptake of 5.35 mmol g −1 at 273 K and 1 bar CO 2 partial pressure. Density functional theory calculations suggest that the high CO 2 uptake performance of the HMCNs is associated with the chemical modification of the surface, as a result of N- and O- co-doping. When assembled in a supercapacitor , 3/2-HMCNs-900 exhibits a high specific capacitance (475 F g −1 at 1.3 A) and a fast charge-discharge rate of 13.3 F s −1 g −1 . This study presents a novel, resource-efficient and environmentally friendly method for preparing HMCNs for energy and environmental applications.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Meng-Ke Hu,Shenghua Zhou,Dong-Dong Ma,Qi-Long Zhu
The heterogenized metallomacrocycles with atomically dispersed active sites are identified as the promising candidates for electrocatalytic CO 2 reduction reaction (CO 2 RR), where their unique heterointerface with interaction between sp 2 carbon and macrocyclic molecules is important but remains vague. Herein, based on well-structured nickel phthalocyanine and porphyrin with the same functional groups (MeNiPc and MeNiPp), the influences of heterointerfacial effect on catalytic performances are systematically disclosed. Through the molecular structure-induced self-adaptive adsorption with optimized heterointerfacial distance, MeNiPc/graphene reveals a high CO Faradaic efficiency of ~99% in a wide potential window, greatly outperforming the MeNiPp/graphene counterpart (≤29.6%). Detailed measurements and theoretical calculations decipher that the higher CO 2 RR activity of MeNiPc/graphene is attributed to the unique electronic structures of the Ni-N 4 configurations suitable for well-suited heterointerfacial charge transfer and rapid CO desorption. Additionally, the extended research confirms the universality of heterointerface engineering on boosting the catalytic performances.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jie Qi,Xiaojiang Li,Xin Lv,Yang Ge,Jinyu Wang,Hongsheng Lu
Wax precipitation leads to destructive harms in the exploitation and transportation of petroleum. Solvent treatments can remove paraffin wax easily but the separation of solvent relying on distillation is admitted inefficient. Aiming at enhancing the separation and recovery performance of paraffin wax, CO 2 -responsive emulsion (SHS/W emulsion) based on switchable hydrophilicity solvents (SHS) is adopted. Since the paraffin wax is dissolved, emulsified, and dispersed by SHS/W emulsion, SHS/W emulsion exhibits better removal performance than SHS. The paraffin wax is recovered effectively upon introducing CO 2 , which attributes to the transformation of SHS from hydrophobic to hydrophilic state. Compared with the SHS system, the recovery of paraffin wax is improved obviously by introducing surfactant Span80. Owing to the deprotonation of SHS by bubbling N 2 and heating, 77.6% SHS is recycled after recovering paraffin wax. Here, the recycled SHS can be used to realize the removal of paraffin wax again. Thus, it is a promising and alternative strategy for realizing the sustainable and rapid removal of paraffin wax in the petroleum industry.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Meng Zhao,Yujie Ban,Weishen Yang
Ionic liquid molecule layers (ILMLs) were assembled on MOF-808 with high porosity for gas adsorption. ILMLs, as a result of better affinity to CO 2 , perform like an adhesive layer to trap CO 2 and MOF-808 performs as a gas reservoir. Deliberately controlling the thickness of ILMLs from 1.7 to 18 nm, we strike a balance of capacity, selectivity and cycling performances for CO 2 capture. The optimal composite adsorbs substantial amount of CO 2 at ambient conditions (3.00 mmol g −1 ), which is 2.6 times of that on MOF-808 (1.15 mmol g −1 ). CO 2 /N 2 selectivity towards mimic combustion flue gas in industry, was 372 (towards 15 mol.% of CO 2 in N 2 ) and 478 (towards 5 mol.% of CO 2 in N 2 ), near one-order magnitude higher than MOF-808 and exceeding most benchmark materials. Notably, by overcoming the gas–liquid interface limitation, CO 2 capacity on each gram of ILMLs was 1000 times higher than that of the bulk liquid. The composite presents cycling separation performances with great energy efficiency for mimic flus gas, as a complete regeneration can be freely achieved at ambient temperature.
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2022
·
IF 16.383
Baopeng Yang,Kang Liu,HuangJingWei Li,Changxu Liu,Junwei Fu,Hongmei Li,Jianan Erick Huang,Pengfei Ou,Tartela Alkayyali,Chao Cai,Yuxia Duan,Hui Liu,Pengda An,Ning Zhang,Wenzhang Li,Xiaoqing Qiu,Chuankun Jia,Junhua Hu,Liyuan Chai,Zhang Lin,Yongli Gao,Masahiro Miyauchi,Emiliano Cortés,Stefan A. Maier,Min Liu
Electrochemical CO2 reduction is a promising way to mitigate CO2 emissions and close the anthropogenic carbon cycle. Among products from CO2RR, multicarbon chemicals, such as ethylene and ethanol with high energy density, are more valuable. However, the selectivity and reaction rate of C2 production are unsatisfactory due to the sluggish thermodynamics and kinetics of C–C coupling. The electric field and thermal field have been studied and utilized to promote catalytic reactions, as they can regulate the thermodynamic and kinetic barriers of reactions. Either raising the potential or heating the electrolyte can enhance C–C coupling, but these come at the cost of increasing side reactions, such as the hydrogen evolution reaction. Here, we present a generic strategy to enhance the local electric field and temperature simultaneously and dramatically improve the electric–thermal synergy desired in electrocatalysis. A conformal coating of ∼5 nm of polytetrafluoroethylene significantly improves the catalytic ability of copper nanoneedles (∼7-fold electric field and ∼40 K temperature enhancement at the tips compared with bare copper nanoneedles experimentally), resulting in an improved C2 Faradaic efficiency of over 86% at a partial current density of more than 250 mA cm–2 and a record-high C2 turnover frequency of 11.5 ± 0.3 s–1 Cu site–1. Combined with its low cost and scalability, the electric–thermal strategy for a state-of-the-art catalyst not only offers new insight into improving activity and selectivity of value-added C2 products as we demonstrated but also inspires advances in efficiency and/or selectivity of other valuable electro-/photocatalysis such as hydrogen evolution, nitrogen reduction, and hydrogen peroxide electrosynthesis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Kejun Chen,Maoqi Cao,Ganghai Ni,Shanyong Chen,Hanxiao Liao,Li Zhu,Hongmei Li,Junwei Fu,Junhua Hu,Emiliano Cortés,Min Liu
Nickel phthalocyanine (NiPc) can be at first glance a compelling catalyst for CO 2 reduction reaction (CO 2 RR) because of its Ni–N 4 site. Unfortunately, the pristine NiPc possesses a low catalytic activity resulting from the poor CO 2 adsorption and activation capabilities of the electron-deficiency Ni site. Herein, we develop nickel polyphthalocyanine (NiPPc) with extended conjugation to tailor the electronic density at the Ni active site. The enlarged π conjugation of NiPPc evokes the d-electrons localization, increasing the electronic density at the Ni site, which enhances its CO 2 adsorption and activation. Consequently, NiPPc supported on carbon nanotubes (NiPPc/CNT) in a flow cell delivers an excellent activity of −300 mA cm −2 for CO 2 RR with the CO selectivity of 99.8%, which is much higher than that of NiPc dispersed on carbon nanotubes. NiPPc/CNT exhibits an outstanding stability for CO 2 RR of more than 30 h at a current density of −100 mA cm −2 with an ultrahigh selectivity for CO, exceeding 99.7%. This work showcases a new way of tuning the electronic density of catalytic sites.
✓ 已验证
产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Zhengjun Gu,Xinmei Wang,Pu Huang,Yu Huang,Xuan He,Xinzheng Wei,Jiahe Yue,Juncheng Jiang,Chuanwen Zhao
The rapid cleanup of endogenous CO 2 has become a necessity in environmental control and life support systems (ECLSSs), to ensure crew safety and long-term task execution. The extensively used non-regenerable LiOH and soda lime adsorbents, although exhibit high CO 2 storage capacities and fast kinetics, can hardly fulfill the demands of reduced launch weight and storage volume in the space- and load-limited ECLSSs. New CO 2 adsorbents with desirable attributes including high CO 2 uptakes, good selectivity , facile regeneration, fast adsorption and desorption kinetics, and good multicycle stability are urgently needed. We developed amine-functionalized adsorbents by loading tetraethylenepentamine (TEPA) on mesoporous supports of activated carbon (AC), aluminum oxide (AO) and silica gel (SG). The adsorbents were characterized by N 2 adsorption-desorption, thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), and scanning electron microscope (SEM) to study their microstructural properties. CO 2 adsorption capacities and kinetic performance of the adsorbents with different supports and various amine loadings (10–50 wt%) were evaluated in 2%CO 2 at 20 °C. The effects of support and amine loading on the structure-performance relationships of the adsorbents were demonstrated. The TEPA-SG-20 adsorbent (20 wt% TEPA loaded on silica gel support) exhibits the highest CO 2 adsorption capacity of 1.90 mmol CO 2 /g and the maximum amine efficiency of 0.48 mmol CO 2 /mmol N. TEPA-SG-20 also exhibits fast CO 2 adsorption kinetics , and the Avrami fractional order kinetic model provides a satisfactory correlation of the experimental CO 2 uptakes. Furthermore, the TEPA-SG-20 adsorbent can be efficiently regenerated at 110 °C with a great regeneration efficacy of 97%. The desired adsorbent also exhibits good working stability with a low loss-in-capacity of 4.32% in 10 consecutive cycles. The good CO 2 adsorption performance of TEPA-SG-20 is associated with the excellent microstructural properties such as high surface area, great pore volume and uniform dispersion of amine species. Overall, the desired TEPA-SG-20 adsorbent shows promise for low-concentration CO 2 removal in ECLSSs.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2022
·Vol. 105
·期 6
·3729-3734
·
IF 4.186
Wei Li,Yanan Sun,Li Ye,Weijian Han,Fenghua Chen,Jianling Zhang,Tong Zhao
Subjected to the manufacturing methods (sputtering or mechanochemical synthesis), the reported high entropy nitrides (HENs) were limited to the forms of coating and powder. Here, we report a novel strategy in preparing HEN ceramic nanofibers (HENCNFs) from liquid precursor via electrospinning followed by high-temperature NH 3 atmosphere nitridation. The as-prepared HENCNFs include five uniform dispersed metal elements, Ti, Hf, Nb, Ta, and Mo, and have a single face-centered cubic structure. Interestingly, the obtained HENCNFs show photocatalyst activity in CO 2 reduction. The product selectivity of photocatalytic CO 2 reduction reaction is 96.4%, and no performance degradation was detected during five cycles photocatalysis test.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）