APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Ke Ye,Tianfu Liu,Yanpeng Song,Qi Wang,Guoxiong Wang
Electrochemical CO 2 reduction reaction (CO 2 RR) offers an appealing route to simultaneously store intermittent renewable energy as value-added chemicals and close carbon cycle. Silver (Ag) catalyst is a promising candidate for the electrochemical conversion of CO 2 to CO, but the electrocatalytic properties are still insufficient for practical applications. Herein, we put forward a strategy to in situ reconstruct a heterogeneous Ag 2 S/Ag interface structure, in which their strong interactions facilitate CO 2 RR performance. The in situ reconstructive Ag 2 S/Ag catalyst achieves a large current density of 421.7 ± 14.4 mA cm –2 at –0.70 V vs . reversible hydrogen electrode (RHE) and maintains steadily at a current density of 244.5 ± 31.8 mA cm –2 and CO Faradaic efficiency of 99.1 ± 0.8 % at –0.49 V vs . RHE for 50 h, superior to state-of-the-art CO-selective Ag-based catalysts. Density functional theory calculations reveal that the in situ reconstructive Ag 2 S/Ag interface active sites stabilize the *COOH intermediate during CO 2 RR process.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 10
·3422-3427
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IF 6.119
Yuqing Shao,Xinkui Wang,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Pang,Qiang Xu,Min Ji,Min Wang
Solar-driven CO2 conversion into fuels and sustainable energy has attracted increasing attention around the world. However, the efficiency of the transformation remains relatively low due to the rapid recombination of photogenerated charge carriers. In this work, we prepared a ZnIn2S4–ZnAlOx nanocomposite for visible light driven CO2 reduction. The thin layered structure facilitated the photoinduced charge carrier separation and transfer, and also gave excellent adsorption ability towards CO2 molecules. Such a nanocatalyst exhibited excellent activity in visible-light driven CO2 reduction with a CO optimal formation rate of 1100 μmol g−1 h−1, which is 5 times that over bulk ZnIn2S4, and the CO/H2 ratio was increased from 0.2 over bulk ZnIn2S4 to 1.5 over the ZnIn2S4–ZnAlOx composite. In situ FT-IR experiments indicated that CO2 was reduced on ZnIn2S4–ZnAlOx following a COOH* pathway. This work gives insights into the mechanism of the photocatalytic CO2 reduction reaction and inspiration to construct novel heterostructure materials for application in energy and environmental catalysis.
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ACS Applied Nano Materials
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2021
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IF 5.097
Zhi Liu,Jia Zheng,Lianfeng Duan,Zhi Zhu
CO2 photoreduction into high-valued fuels is considered as a promising route to alleviate the clash between the environment and energy. Morphology-dependent CeO2 nanocrystallines with special crystal planes and increased amounts of specific surface areas, structural defects, and active sites have recently demonstrated excellent performance in catalysis. In this article, a biomass-assisted synthesis of CeO2 (BC) photocatalyst is successfully synthesized via a simple yet effective hydrothermal-calcining method by using commercial Ce(NO3)3 as a precursor and leaves of Alternanthera philoxeroides (LAP) as a crystal growth modifier. The amount of LAP introduced into the precursor has a significant effect on regulating the growth of the formed CeO2 from nanocubes to nanorods for the resulting BCs. Owing to the emergence of the just right microenvironment for regulating the growth of the CeO2 nanocrystalline, the optimal sample of BC-15 with a morphology of nanorods is found to be the most efficient one as a photocatalyst for CO2 reduction under visible light. As the major product, the CO yield (126.8 μmol g–1 at a reaction time of 6 h) of BC-15 is ∼7.4-fold of the reference CeO2 nanocubes synthesized without LAP in the precursor. In addition, the underlying evolution process of the nanorods and detailed mechanism insight into the boosted CO2 photoreduction performance are investigated by means of a series of experimental characterizations and results. The present work provides a meaningful protocol to utilize the crystal phase engineering strategy to design morphology dependence of photocatalysts and assisted synthesis with renewable biomass materials for solar-to-fuel conversion.
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RSC Advances
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2021
·Vol. 11
·期 4
·2040-2046
·
IF 3.361
Yang Liu,Xin Liang,Jie Zhang,Jimmy Yun,Zuobo Yang
In this study, monodispersed NiRu nanocrystals with a diameter of 3 nm were synthesized at 90 °C via a tuning hot-inject method to lower the temperature of the organic phase synthesis of monodispersed nanomaterials. The key factor for the nanocrystalline formation of NiRu alloy nanocrystals was summarized in detail. Simultaneously, the synergistic effect of Ni and Ru in CO2 methanation was explored. Doping trace Ru can significantly improve the conversion rate of CO2 methanation and CH4 selectivity. The underlying mechanism was studied in detail via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed hydrogen reduction (H2-TPR) and desorption (H2-TPD) tests, and temperature-programmed desorption of CO2 (CO2-TPD). This study gives out a new way for the general synthesis of monodisperse nickel-based nanocrystals and provides a reference for the development and application of monodispersed nanoparticles for CO2 methanation.
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高影响因子
ACS Catalysis
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2021
·
IF 13.084
Tian-Wen Jiang,Ya-Wei Zhou,Xian-Yin Ma,Xianxian Qin,Hong Li,Chen Ding,Bei Jiang,Kun Jiang,Wen-Bin Cai
The electrochemical CO2 reduction reaction (CO2RR) on Pd-based electrodes to dissolved formate and/or gaseous CO is largely dependent on potential and the electrode material, yet there is a lack of molecular-level insights into this dependence. Herein, in situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) in conjunction with differential electrochemical mass spectrometry (DEMS), gas chromatography (GC), and nuclear magnetic resonance (NMR) measurements is applied to investigate the CO2RR on Pd and Pd-B film electrodes, providing a direct observation of the role of surface CO as well as the B-doping effect at varied potentials. Comprehensive spectrometric results reveal that at lower overpotentials, CO gradually accumulates on both Pd electrode surfaces poisoning the dominant formate pathway, while at higher overpotentials, surface CO forms facilely with linearly bonded CO (the minor surface CO species) acting as an active precursor and bridge-bonded CO (the major surface CO species) as a spectator toward the gaseous CO product. Moreover, B-doping in Pd hinders CO formation and promotes formate production on the Pd-B electrode for the CO2RR as compared to that on the pristine Pd electrode at all of the overpotentials under investigation.
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ACS Applied Energy Materials
·
2020
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IF 4.473
Zhongkai Xie,Yuyan Xu,Di Li,Suci Meng,Min Chen,Deli Jiang
The highly efficient spatial carrier separation and abundant active sites are significant for CO2 photocatalytic reduction efficiency. Herein, an ultrathin Bi2O3 nanosheet/Bi2WO6 network heterostructure is successfully synthesized via a covalently bonded epitaxial growth strategy. Due to cosharing of the Bi–O tetrahedron between Bi2O3 and Bi2WO6, this heterostructure exhibits a compact interface, which can provide a highway for the charge transfer and then boost their separation. Moreover, the pores generated from the hierarchical structure afford abundant exposed photocatalytic active sites. Thus, the optimal Bi2O3/Bi2WO6 heterostructure (BOBWO-12) shows superior photocatalytic performance for CO2 reduction with an ultrahigh selectivity as well as the removal of RhB. Notably, the photocatalytic CO generation rate over BOBWO-12 reaches up to 17.39 μmol·g–1·h–1, which is 18.0 and 4.2 times higher than that of bulk-Bi2WO6 and Bi2WO6 nanosheets, respectively, and the selectivity is of about 95.4%. Moreover, the Bi2O3/Bi2WO6 heterostructure also exhibits improved long-term stability, resulting from the firm heterointerface. Our studies present a conventient avenue to construct a high-efficiency heterostructure photocatalyst with a firm interface by the covalently bonded epitaxial growth method for CO2 reduction.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Tianjiao Wang,Hongyan Yao,Ningning Song,Yanchao Yang,Kaixiang Shi,Shaowei Guan
In recent years, linear polyimides of intrinsic microporosity have been widely used in the field of gas adsorption and separation because of their high BET surface area and microporous structures. Most of the microporous structures come from the twisted main-chain structures in the linear polyimides of intrinsic microporosity. Therefore, most linear polyimides (PI) without twisted structure have no porosity. Herein, to construct the linear polyimide with microporous structure, a sequence of microporous polyimides (PIs-CL) were constructed from the flexible linear polyimide precursors through the thermal crosslinking reaction. The polyimide precursors without twisted structure were synthesized from a well-designed diamine TFVBPA with cross-linkable ethynyl groups and several commercial dianhydrides (ODPA, BPDA, PMDA and 6FDA) by polycondensation to research the influence of the main-chain structure on the porous characters. The introduction of crosslinked structures gives the linear crosslinked polyimides (PIs-CL) with porous structures. The PIs-CL show obviously improved porosity (0.52–1.71 nm) and higher BET surface area (337–618 m 2 g −1 ) than those of the uncrosslinked polyimides (PIs). Moreover, PIs-CL have favorable CO 2 adsorption (5.7–9.3 wt%) as well as good CO 2 /N 2 selectivity (34.4–58.5) at 273 K, which are better than other polyimides materials. The introduction of crosslinked structures is an effective way to improve microporous porosity and gas sorption performance.
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CATALYSIS TODAY
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2020
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IF 5.825
Junhui Liu,Guanghui Zhang,Xiao Jiang,Junhu Wang,Chunshan Song,Xinwen Guo
Iron-based catalysts have been widely used to synthesize value-added hydrocarbons through CO 2 hydrogenation. Fe carbide, Fe 5 C 2 , was proposed as the active phase responsible for C C coupling during the chain growth. However, the reaction mechanism over iron-based catalysts is still under debate due to the presence of multiple phases of Fe species. In this work, Fe 5 C 2 and K-modified Fe 5 C 2 were prepared and used to study the relationship between the Fe phase, catalytic performance and reaction pathways. CH 4 and CO selectivities of 46.1 C-mol% and 2.8 C-mol% were obtained on Fe 5 C 2 at a CO 2 conversion of 49.8 %, with the main hydrocarbon products being alkanes. With the addition of the promoter K, the C 2 -C 4 = selectivity increased to above 38.0 C-mol%, and the selectivity to C 5+ hydrocarbons increased to 23.9 C-mol% at a similar CO 2 conversion. CH 4 and C 2+ hydrocarbons formed through the CO 2 →CO→hydrocarbons (indirect) route over K-modified Fe 5 C 2 , whereas the direct hydrogenation route occurred on unmodified Fe 5 C 2 in addition to the indirect route of CO 2 to CO to hydrocarbons through Fischer-Tropsch synthesis (FTS) processes. This work offers insights in direct CO 2 hydrogenation over Fe 5 C 2 and Fe 3 O 4 -Fe 5 C 2 catalysts, which advances the understanding of the functions of active phases and reaction pathways of CO 2 hydrogenation over iron-based catalysts.
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JOURNAL OF CATALYSIS
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2020
·
IF 7.888
Lan Yuan,Yue-Hua Li,Zi-Rong Tang,Jinlong Gong,Yi-Jun Xu
Pairing CO 2 reduction with oxidative organic synthesis in one photoredox cycle opens a new avenue for cooperative utilization of excited electrons and holes towards efficient solar-to-chemical energy conversion. In this work, we demonstrate a facile cetyltrimethylammonium bromide (CTAB) surfactant functionalized ZnIn 2 S 4 (ZIS)-based dual-functional reaction system for efficient visible light-driven CO 2 -to-CO conversion pairing with selective oxidation of benzyl alcohol to value-added C C coupled products. Our research suggests that the markedly enhanced redox activities are mainly attributed to the unique structure of CTAB-ZIS featuring more crystalline and surface defects, which greatly promotes the interfacial charge carrier transfer, and in particular elevates CO 2 activation and electrons reducibility. It is anticipated that this work would inspire further establishment of efficient novel photocatalysts and cooperative reaction system coupling CO 2 reduction and organic synthesis in a cost-effective manner under ambient conditions to meet the economic and social sustainability goals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Wei Wang,Yunlei Zhong,Xinyu Zhang,Sainan Zhu,Yourong Tao,Yanxin Zhang,Hongsen Zhu,Yifei Zhang,Xingcai Wu,Guo Hong
Surface self-reconstruction by the electrochemical activation is considered as an effective strategy to increase the oxygen evolution reaction (OER) performance of transition metal compounds. Herein, uniform Co 2 (OH) 3 Cl microspheres are developed and present an activation-enhanced OER performance caused by the etching of lattice Cl − after 500 cyclic voltammetry (CV) cycles. Furthermore, the OER activity of Co 2 (OH) 3 Cl can be further enhanced after small amounts of Fe modification (Fe 2+ as precursor). Fe doping into Co 2 (OH) 3 Cl lattices can make the etching of surface lattice Cl − easier and generate more surface vacancies to absorb oxygen species. Meanwhile, small amounts of Fe modification can result in a moderate surface oxygen adsorption affinity, facilitating the activation of intermediate oxygen species. Consequently, the 10% Fe-Co 2 (OH) 3 Cl exhibits a superior OER activity with a lower overpotential of 273 mV at 10 mA cm −2 (after 500 CV cycles) along with an excellent stability as compared with commercial RuO 2 .
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JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Youxu Yu,Fengjia Xie,Rong Chen,Xun Zhu,Qiang Liao,Dingding Ye,Jinwang Li,Sihong Song
The objective of this work is to explore the role of CO 2 in the photocatalytic fuel cell with TiO 2 as the photoanode and methanol as a fuel under acid condition by making the anode electrolyte saturated with CO 2 . It is interesting to find that the performance of the photocatalytic fuel cell can be improved at low methanol concentration in the presence of CO 2 . This is probably because TiO 2 has an adequate conduction band for photocatalytic reduction of CO 2 to organics at the photoanode, which increases the methanol concentration at the catalytic surface to alleviate the mass transfer issue encountered in the low methanol concentration operation, and hinders the recombination of the electron-hole pairs. Moreover, the methanol concentration at the outlet of the photoanode can be even higher than the supplied methanol concentration. However, this effect is weakened and even disappears as the supplied methanol concentration increases. This work gives new insights into the role of CO 2 in the photocatalytic fuel cell with the photoanode having an adequate conduction band for photocatalytic reduction of CO 2 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Xiahui Lin,Yilin Gao,Min Jiang,Yongfan Zhang,Yidong Hou,Wenxin Dai,Sibo Wang,Zhengxin Ding
Herein, we report the facile synthesis of uniform perovskite hydroxide CoSn(OH) 6 nanocubes and their first use as noble-metal-free, highly efficient and stable catalysts for the deoxygenative reduction of CO 2 to CO with visible light. The CoSn(OH) 6 sample is synthesized through a one-pot co-precipitation method and fully characterized by various techniques including XRD, FTIR, FESEM, TEM, EDX, EDX-mappings, XPS, DRS, and N 2 sorption measurements. The CoSn(OH) 6 solid is found by theoretical calculations to be capable of absorbing and activating CO 2 molecules on the (100) surface. Under the optimal reaction conditions, the CoSn(OH) 6 catalyst exhibits a high CO 2 reduction activity with visible light irradiation, affording a CO generation rate of 18.7 μmol h −1 . The stability and reusability of the CoSn(OH) 6 catalyst for photocatalytic CO 2 reduction are solidly confirmed. Results of in situ photoluminescence spectroscopy and photocurrent response characterizations indicate that the CoSn(OH) 6 catalyst can efficiently promote the separation and transfers of photoexcited charge carriers during photocatalysis, and eventually leading to obviously enhanced CO 2 photoreduction performance. Moreover, a possible mechanism for the photocatalytic CO 2 reduction reaction is also proposed based on the results of activity evaluation and photo-/electro-chemical measurements.
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