Journal of Physical Chemistry C
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2022
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IF 4.177
Yanjun Yu,Chen Chen,Yiheng Liu,Hongliang Yu,Shuaijie Li,Yanan Xue,Ning Cai,Jianzhi Wang,Faquan Yu
Developing efficient and cost-effective bifunctional catalytic electrodes is of great importance to water splitting. In this study, hybrid Ni/Ni(OH)2-coated NiCo2O4 nanorods were grown on Ni foam (NF) by a facile growth–conversion–epitaxy approach. The epitaxial decoration of Ni/Ni(OH)2 composite could increase the intrinsic activity of NiCo2O4/NF and enhance the charge-transfer rate. This self-standing hierarchical nanohybrid with unique surface chemistry and interface engineering exhibits an excellent electrocatalytic performance. The optimized Ni/Ni(OH)2-NiCo2O4/NF only requires overpotentials of 53 and 235 mV to reach a current density of 10 mA cm–2 for HER and OER, respectively. The electrolyzer achieved 10 mA cm–2 at a low cell voltage of 1.51 V for water splitting. This work offers a new perspective for rationally designing electrocatalytic materials by surface decoration.
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Frontiers in Bioengineering and Biotechnology
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2022
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IF 6.064
Lv Xianqing,Luo Xiaolin,Cheng Xin,Liu Jing,Li Changzhi,Shuai Li
Hydroxymethylfurfural (HMF) derivatives such as 2,5-bis(hydroxymethyl)furan (BHMF) and furandicarboxylic acid (FDCA) are promising alternative of fossil-based diols and dicarboxylic acids for synthesis of polyesters such as polyethylene terephthalate (PET). However, high cost for preparing HMF from biomass discourages the commercialization of HMF-derived polyesters. Since producing furfural (FUR) from five-carbon sugars (e.g., xylose) via dehydration is an inexpensive and commercialized process, we herein reported a method to synthesize BHMF derivatives (5-(ethoxymethyl)furan-2-methanol (EMFM), 2,5-bis(hydroxymethyl)furan monoacetate (BHMFM) and 2,5-bis(hydroxymethyl)furan diacetate (BHMFD) from furfural derivatives, i.e., (2-(ethoxymethyl)furan (EMF) and furfuryl acetate (FA)). To avoid strong acid-induced side reactions (e.g., furan ring opening, condensation and carbonization), two reaction systems, i.e., a low-concentration HCl aqueous solution combined with formaldehyde and anhydrous acetic acid combined with paraformaldehyde, were found to be suitable for such a hydroxymethylation reaction and could lead to decent product yields. In order to improve the carbon utilization, condensed furanic byproducts were further converted into hydrocarbon fuels via a reported two-step hydrodeoxygenation (HDO) process. This study not only validates the possibility of synthesizing functional HMF derivatives (EMFM, BHMFM, and BHMFD) from commercially-available FUR derivatives (EMF and FA), but also provide a new way to transform condensed furanics to value-added hydrocarbon fuels.
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Sustainable Energy & Fuels
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2022
·Vol. 6
·期 6
·1616-1624
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IF 6.813
Haofei Gao,Fengan Han,Guangyi Li,Aiqin Wang,Yu Cong,Zhizhou Li,Wei Wang,Ning Li
In this work, jet fuel range high-density polycycloalkanes, dicyclohexylmethane and dodecahydrofluorene, were first synthesized by a two-step method with vanillin and cyclohexanone, two platform compounds that can be derived from lignin. In the first step, 2-(4-hydroxy-3-methoxybenzylidene)cyclohexan-1-one, a jet fuel range C13 polycycloalkane precursor, was obtained through an acid-catalyzed aldol condensation reaction between vanillin and cyclohexanone over a series of titanium dioxide based nanometer material catalysts. Among them, sulfated titania nanofibers (STNFs) exhibited the highest activity. Over them, a high yield (81%) of 2-(4-hydroxy-3-methoxybenzylidene)cyclohexan-1-one was obtained after the reaction was carried out at 423 K for 10 h. On the basis of the characterization results, the good performance of the STNF catalyst can be attributed to its higher acid strength and higher Brønsted to Lewis acid site ratio. Subsequently, the aldol condensation product was further converted to a mixture of dicyclohexylmethane and dodecahydrofluorene by hydrodeoxygenation (HDO) under the co-catalysis of Pd/C and H-Y zeolite. According to our measurement, the cycloalkane mixture as obtained from the HDO process has a higher density (0.95 g mL−1) and lower freezing point (256 K). As a potential application, it can be blended into low freezing point jet fuels to improve their volumetric heat values.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Rui-Min Sun,Qi-Dong Ruan,Jiu-Ju Feng,Lu Zhang,Ai-Jun Wang
Developing efficient and highly low-cost electrocatalysts for oxygen reduction reaction (ORR) is highly desirable and challenging for renewable energy devices. In this work, a novel sandwich-like heterostructured nanocomposite was facilely constructed via incorporation of Co 9 S 8 nanoclusters/Co 3 [Co(CN) 6 ] 2 nanocubes in N,S-doped carbon multilayers (Co 9 S 8 /Co 3 [Co(CN) 6 ] 2 /N,S-CMLs) by a one-pot coordination-modulated pyrolysis of a mixture containing dicyandiamide, Co(NO 3 ) 2 and Evans blue at 800 °C. The control tests demonstrated critical roles of the pyrolysis temperature played on the final morphology and shape, and discussed the formation mechanism in detail. The as-prepared catalyst exhibited appealing electrocatalytic performance for ORR with a more positive onset potential ( E onset = 0.96 V vs. RHE) and half-wave potential ( E 1/2 = 0.87 V vs. RHE) in 0.1 M KOH electrolyte, far outperforming other home-made catalysts and commercial Pt/C. This work opens a new avenue to prepare efficient, cost-effectiveness and stable electrocatalysts in sustainable energy storage and conversion devices.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yunni Liu,Qian Li,Zichao Lian,Jinchen Fan,Ying Tao,Guisheng Li,Hexing Li
Polarization field introduced photoelectrocatalytic system has been raised and applied for environmental purification and green fuel generation. Herein, we synthesized the Ag 2 O/TiO 2 nanotubes arrays (TNTs) p - n heterojunction photoanodes and innovatively introduced the SrTiO 3 (STO) as a relay to construct a highly stable PEC system. The SrTiO 3 layers with the ferroelectric properties were inserted in the interfaces between p-Ag 2 O and n-TiO 2 , creating a charge-stable polarized electric field thereby maintaining a constant driving force that promoted the effctive separation of electron and hole between SrTiO 3 and TNTs, and prevented the electron transfer from SrTiO 3 to Ag 2 O. Controlling suitable annealing and regulating hydrothermal time could induce SrTiO 3 spontaneous polarization, resulting in effective photoinduced charge separation. Consequently, the as-designed TNTs/STO/Ag 2 O photoanodes exhibited excellent PEC activity and stability (>40 h) for both persistent organic pollutants degradation and synergistic hydrogen evolution owing to the strengthened charge carrier capture ability of solar light and improved photocurrent density.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Lingxin Peng,Liang Su,Xu Yu,Rongyan Wang,Xiangzhi Cui,Han Tian,Shaowen Cao,Bao Yu Xia,Jianlin Shi
Developing efficient electrocatalysts is of significance for hydrogen production in acid electrolyte. In this work, we report a facile decoration of ruthenium species onto tungsten oxides to construct the Mott-Schottky heterojunction electrocatalyst for hydrogen evolution. The resultant Ru-WO 2.72 hybrid exhibits a superior Ru-based mass activity of 161.6 times higher than that of commercial Ru/C for hydrogen evolution, featuring a Tafel slope of 50 mV dec −1 and 40 mV overpotential at the current density of 10 mA cm −2 . The uniform distribution of Ru species triggers a strong electron transfer across the Ru-WO 2.72 Schottky barrier, resulting in a largely increased local electron density on the active Ru surface. Such electron enrichment induced by the Mott-Schottky effect at the metal-metal oxides interface is responsible for enhanced hydrogen production. This work demonstrates an effective strategy by Mott-Schottky effect to regulate electron distribution, which would evoke more inspiration in designing efficient electrocatalysis and beyond.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Boxuan Yang,Xian Li,Zhongqiu Hua,Zhemin Li,Xiangnan He,Rui Yan,Yanhao Li,Zinan Zhi,Chen Tian
Agricultural activities produce substantial amounts of ammonia (NH 3 ), affecting agricultural ecology and resulting in environmental pollution. NH 3 detection based on sensor technology in the field has long been a challenging topic. Detection can be hampered by multiple interfering gases, as well as fluctuations in temperature and humidity, which can cause signal failure. Here, a simple and systematized NH 3 monitor coupled with a differential catalytic conversion method was designed to efficiently and continuously monitor NH 3 , independently of changes in the external environment. Overall, the catalytic conversion method of NH 3 into NO 2 increased the recognition of NH 3 and excluded most interfering gases. With the addition of differential processing , the detection results were further refined by eliminating the influence of oxidizing interfering gases, temperature, and humidity. This method can be applied in various demanding environments to obtain accurate results and eliminate the background interference that has long plagued sensor research.
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Processes
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2022
·Vol. 10
·期 4
·668
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IF 3.352
Ruigan Hu,Fuyue Liu,Haoqi Qiu,He Miao,Qin Wang,Houcheng Zhang,Fu Wang,Jinliang Yuan
The progress of high-efficiency non-precious metal anode catalysts for direct seawater splitting is of great importance. However, due to the slow oxygen evolution reaction (OER) kinetics, competition of chlorine evolution reaction (ClER), and corrosion of chloride ions on the anode, the direct seawater splitting faces many challenges. Herein, we develop a perovskite@NiFe layered double hydroxide composite for anode catalyst based on Ba0.5Sr0.5Co0.8Fe0.2O3(BSCF) and NiFe layered double hydroxide (NiFe-LDH) heterostructure. The optimized BSCF@CeO2@NiFe exhibits excellent OER activity, with the potential at 100 mA cm−2(Ej = 100) being 1.62 V in the alkaline natural seawater. Moreover, the electrolytic cell composed of BSCF@CeO2@NiFe anode shows an excellent stability, with negligible attenuation during the long-term overall seawater splitting with the remarkable self-recovery ability in the initial operation stage, and the direct seawater splitting potential increasing by about 30 mV at 10 mA cm−2. Our work can give a guidance for the design and preparation of anode catalysts for the direct seawater splitting.Keywords:seawater electrolysis;perovskites;layered double hydroxide;oxygen evolution reaction;anode catalysts
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yun Wu,Rui Yao,Qiang Zhao,Jinping Li,Guang Liu
The development of high-performance and durable Ru-based electrocatalysts in proton exchange membrane (PEM) water electrolyzers for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) remains a huge challenge due to the severe catalyst’s corrosion and high reaction overpotential in acid media. Herein, we reported a synergistic strategy of effectively combining hetero-atom doping and oxygen vacancy in the La-doped RuO 2 nanocrystals, successfully realized by a hydrothermal and followed annealing process aiming for efficiently overall water splitting. The as-obtained La-doped RuO 2 nanocrystals demonstrate superior electrocatalytic performances with ultra-low overpotential of 208 mV for OER and 71 mV for HER at the current density of 10 mA/cm 2 together with robust long-term stability in 0.5 M H 2 SO 4 electrolyte, which are 222 and 15 mV lower in overpotentials than that of bare RuO 2 electrocatalyst. Moreover, the La-doped RuO 2 nanocrystals only require a cell voltage of 1.53 V to drive the overall water splitting reaction and exhibit a remarkable stability. Density functional theory (DFT) calculations further reveal that the synergistic effect of La doping and oxygen vacancy engineering could tune the d-band center of Ru active sites and optimize the Gibbs free energy of intermediate state, thus enhancing the activity of RuO 2 . Such synergistic strategy of aliovalent doping and vacancy engineering for much enhanced acid electrocatalysis may offer important referential values for exploring efficient electrocatalysts towards overall water splitting in acidic media.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Zhuo Liu,Fei Guo,Lina Han,Jie Xiao,Xiaoyuan Zeng,Chengxu Zhang,Peng Dong,Mian Li,Yingjie Zhang
Along with the widespread applications of various energy storage and conversion devices, the prices of precious metal platinum (Pt) and transition-metal cobalt/nickel keep continuously growing. In the future, designing high-efficiency nonprecious-metal catalysts based on low-cost iron (Fe) and manganese (Mn) metals for hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) is fairly critical for commercial applications of hydrogen fuel cells. In this study, for the first time, we design novel three-dimensional (3D) hybrid networks consisting of manganese oxide (MnO)-modified, iron carbide (Fe3C)-embedded, and boron (B)/nitrogen (N) codoped hierarchically porous carbon nanofibers (denoted FeMn@BNPCFs). After optimizing the pyrolysis temperatures, the optimal FeMn@BNPCFs-900 catalyst displays the best HER and ORR catalytic activities in an alkaline solution. As expected, the HER onset potential (Eonset) and the potential at a current density of −10 mA cm–2 for FeMn@BNPCFs-900 in 1.0 M KOH are just 36 and 194 mV more negative than the state-of-the-art 20 wt % Pt/C catalyst with more superior stability. In particular, the FeMn@BNPCFs-900 catalyst shows excellent ORR catalytic activity with a more positive Eonset (0.946 V vs RHE), a more positive half-wave potential (E1/2 = 0.868 V vs RHE), better long-term stability, and higher methanol tolerance surpassing the commercial 20 wt % Pt/C (Eonset = 0.943 V vs RHE, E1/2 = 0.854 V vs RHE) and most previously reported precious-metal-free catalysts in 0.1 M KOH. The synergistic effects of 3D hierarchically macro-/mesoporous architectures, advanced charge transport capacity, abundant carbon defects/edges, abundant B (2.3 atom %) and N (4.9 atom %) dopants, uniformly dispersed Fe3C@BNC NPs, and MnO nanocrystallines are responsible for the excellent HER/ORR catalytic activities of the FeMn@BNPCFs-900 catalyst.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhuozheng Hong,Zili Xu,Zhengtao Wu,Hao Zhang,Ping Li,Xun Xu,Shuwang Duo
Tungsten-based nitrides are ideal hydrogen evolution reaction (HER) electrocatalysts owing to their Pt-like electronic structures, high electrical conductivity, and good corrosion resistance. However, the conventional preparation of tungsten-based nitride electrocatalysts suffers from environmentally hazardous sources and high-temperature nitridation processes, which usually restrict HER activity. Herein, we report the direct synthesis of W 2 N on metal–organic framework (MOF)-derived Co-NC microarrays using magnetron sputtering. Co-NC microarray support increased the number of surface activity sites that were exposed to W 2 N. Moreover, the formation of Co-NC@W 2 N Schottky heterojunctions significantly facilitated charge transfer between Co-NC and W 2 N. The Co-NC@W 2 N heterojunctions showed outstanding HER activity with an overpotential of 55 mV in reaching a current density of 10 mA cm −2 . Notably, Co-NC@W 2 N exhibited superior HER performance to Pt/C catalyst at high current densities. This study provides a simple and environmentally friendly approach for fabricating high-performance metal-nitride catalysts for water splitting.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Yu Liu,Yingying Xing,Xinyu Zheng,Shengjie Xu,Di Li,Deli Jiang
Designing high-performance and earth-abundant bifunctional catalysts for electrocatalytic water splitting remains a great challenge. Herein, a novel electrode composed of Cr-doped Co 2 P with P vacancies nanowire arrays (denoted as CrCo 2 P(V p ) NWs) grown on nickel foam was fabricated via a hydrothermal and successive calcination method. The Cr doping and vacancy engineering synergistically enable the exposure of more active sites, optimize electronic structure, and accelerate the charge transport capability, thus enhancing the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performances. As a result, the obtained Cr 0.4 Co 2 P(V p ) NWs catalyst exhibits superior catalytic activities in 1.0 M KOH solution with low overpotentials of 37 mV at −10 mA cm −2 for HER and 253 mV at 20 mA cm −2 for OER, respectively. Furthermore, using Cr 0.4 Co 2 P(V p ) NWs as a dual-function catalyst only requires 1.54 V voltage at 10 mA cm −2 for overall water splitting. Notably, the Cr 0.4 Co 2 P(V p ) NWs catalyst displays satisfactory stability with only a small attenuation of 3.2% after 50 h in a constant current testing. This study highlights the synergistic effect between doping and anion-vacancies in the enhancement of electrocatalytic activities and provides a feasible strategy to design effective, earth-abundant, and stable bifunctional electrocatalysts for water splitting.
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