Solar RRL
·
2023
·Vol. 7
·期 7
·2201093
·
IF 7.9
Xiaohong Ma,Danyang Li,Jun Xie,Jian Qi,Huacheng Jin,Liuyang Bai,Hao Zhang,Feifei You,Fangli Yuan
The reduction of CO 2 to chemical fuel driven by solar energy can not only meet the growing demand for renewable energy, but also balance the carbon cycle in nature. However, the current photocatalysts have low CO 2 conversion due to their poor light capture ability, narrow light response range, and high recombination probability of photogenerated carriers. Herein, a heterogeneous photocatalyst of hollow structured ZnO/ZnS decorated with Pt nanoparticles is synthesized through the hydrothermal process and photodeposition method, showing excellent photocatalytic activity for CO 2 reduction in long-time stability and ≈100% CO selectivity, which can mainly contribute to natural enhanced light-capture ability of the hollow confined space due to multiple reflection and scattering of light in the cavity, thus improving separation efficiency of photogenerated charge carriers due to the type II junction constructed between ZnO and ZnS and the additional reaction active sites after decorating Pt nanoparticles in the surface of the hollow structure.
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CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Zhi-xiu Yang,Xiu Wen,Li-jing Gao,Jin Zhang,Rui-ping Wei,Xiao-mei Pan,Guo-min Xiao
The electrocatalytic carbon dioxide reduction provides a promising route to alleviate the greenhouse effect and energy crisis. We investigated the influencing factors that conversion of CO 2 to C 2 H 4 by preparing Cu 2 O nanoparticles (Cu 2 O-p, Cu 2 O-2p, and Cu 2 O-3p) with exposed different crystal facets, sizes, and grain boundaries. Impressively, the Cu 2 O-3p catalyst exhibits superior selectivity (57.8%) for C 2 H 4 generation due to its abundant {100} & {111} grain boundaries. The study demonstrated that rich grain boundaries have a significant effect on C C coupling for electrocatalysis CO 2 reduction, and offered a learnable route for high-efficient CO 2 reduction catalysts by regulating grain boundary.
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JOURNAL OF MOLECULAR LIQUIDS
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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.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Mengmeng Ni,Lihong Wang,Yao Chai,Bing Wang,Dongmiao Li,Jinni Shen,Zizhong Zhang,Xuxu Wang
The photocatalytic conversion of CO 2 and H 2 O into a series of value-added products is regarded as an important way to mimic natural photosynthesis for solar harvesting. Herein, we prepared CsBi 2 Ta 5 O 16 with a cubic pyrochlore structure via high-temperature molten salt method as a photocatalyst for the first time. The NiO-loaded CsBi 2 Ta 5 O 16 composites could efficiently photocatalyze the conversion of CO 2 into CH 4 and CO, and oxidize H 2 O to O 2 . With 10 wt% NiO loading, the highest yield of CH 4 (7.24 μmol g −1 h −1 ) and O 2 (3.59 μmol g −1 h −1 ) could be achieved. The adsorption and activation of CO 2 molecule on NiO can be attributed to the enhanced CO 2 photocatalytic conversion by the NiO-loaded CsBi 2 Ta 5 O 16 composites. This work provides a design idea of photocatalyst for the full reaction of CO 2 with H 2 O.
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FUEL
·
2022
·
IF 8.035
Xiayi Hu,Juntao Huang,Xinwei He,Qi Luo,Chao'en Li,Changbo Zhou,Rui Zhang
The challenge for the carbon dioxide (CO 2 ) capture by using amine solution is the huge energy cost in solvent regeneration process, this work combined the advantages of three conventional amines, monoethanolamine (MEA), 1-Dimethylamino-2-propanol (1DMA2P), and piperazine (PZ) to formulate an effective trio-amine blend to capture CO 2 , and the results demonstrate that the blends could reduce the energy consumption by 29.4–55.4%, increase the average desorption rate by 60–140%, and increase the cyclic capacity by 40–120%, relative to 5 M MEA solution. Through analysis the regeneration mechanism in detail, it is found that more proton provider in the trio-amine blends could help to reduce the energy consumption by lower the reaction activation energy in the deprotonation process of the protonated amines. Finally compared to the reported amine systems in considering of the energy cost, it is found that the MEA-1DMA2P-PZ could be a potential candidate for capturing CO 2 in industrial.
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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.
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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.
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PubMed
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Lei Wang,Zhiting Zhang,Qi Han,Ying Liu,Junbo Zhong,Jiufu Chen,Jingwei Huang,Houde She,Qizhao Wang
Commercial TiO 2 (P25) is a potentially promising catalyst for photocatalytic CO 2 reduction. Nonetheless, the inefficient light capture ability and egregious charge recombination restrict its further utilization. In this work, CdS and P25 are incorporated to form the composite CdS-P25, which is further immobilized on the surface of a copper-based organic metal framework (MOF), ZIF-67, so as to establish a ternary hybrid CdS-P25/ZIF-67 via a facile hydrothermal method. On the basis of the enhancement in light absorption resulted from the formation of CdS-P25, the incorporation of ZIF-67 further prolongs the light absorption edge of CdS-P25/ZIF-67, up to 552 nm. In addition, the introduction of ZIF-67 with the dual Z-Scheme system constructed could significantly suppress the charge recombination, as revealed by the transient photocurrent value of CdS-P25/ZIF-67, which is 3.47 μA cm −2 , about 20.4 times than that of CdS-P25. Accordingly, the photocatalytic assessment of CdS-P25/ZIF-67 also presents a significantly amelioration in CO 2 reduction reaction (CO 2 RR) in comparison with either CdS-P25 or ZIF-67, giving 1.58 μmol h −1 CH 4 and 1.49 μmol h −1 CO production. Our work sheds light on the investigation of efficacious construction of P25 based hybrids for light-driven photocatalysis.
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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.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Cuihua Ma,Qinghua Li,Zhi Wang,Min Gao,Jixiao Wang,Xingzhong Cao
Polymeric membranes have been widely researched for several decades due to their good processability and low cost. Herein, high-performance thin-film composite (TFC) membranes were prepared by interfacial polymerization using N-methyldiethanolamine (MEDA), 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethylspirobisindane (TTSBI) and trimesoylchloride (TMC). The effects of segmental chain motion on the gas separation performance of the TFC membranes were investigated for the polymeric membranes featuring rigid and contorted sites along the polymer backbone by inducting TTSBI. The results suggested that the introduction of rigid and contorted structures improved the cavities in the membrane, impeded the transport of larger gas, and enhanced the diffusive selectivity. Therefore, the TFC membrane exhibited high permeance and high selectivity with CO 2 permeance of about 1800 GPU and CO 2 /N 2 selectivity of 370 at 0.11 MPa, which is a remarkable improvement in gas separation performance.
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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.
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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.
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