Energy & Environmental Materials
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2023
·
IF 15
Fan Liu,Xinghong Cai,Yang Tang,Wenqian Liu,Qianwei Chen,Peixin Dong,Maowen Xu,Yangyang Tan,Shujuan Bao
Electrocatalytic hydrogen evolution and sulfion (S 2− ) recycling are promising strategies for boosting H 2 production and removing environmental pollutants. Here, a nano-Ni-functionalized molybdenum disulfide (MoS 2 ) nanosheet was assembled on steel mesh (Ni-MoS 2 /SM) for use in sulfide oxidation reaction-assisted, energy-saving H 2 production. Experimental and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS 2 nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH ad , thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction. Meanwhile, the Ni/MoS 2 -based hydrogen evolution reaction + sulfide oxidation reaction system achieved nearly 100% hydrogen production efficiency and only consumed 61% less power per kWh than the oxygen evolution reaction + hydrogen evolution reaction system, which suggested our proposed Ni-MoS 2 and novel hydrogen production system are promising for sustainable energy production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Jieyi Liu,Junde Wei,Xiao Feng,Mingxia Song,Song Shi,Sibao Liu,Guozhu Liu
Hydrodeoxygenation (HDO) is one of the effective methods for upcycling polycarbonate (PC) plastic waste, but the development of low-cost, high-performance HDO catalysts still faces great challenges. In this work, we report that a bifunctional Ni/HZSM-5 catalyst can directly upgrade PC plastic wastes into sustainable aviation fuel ranged cycloalkanes in high yields (99.3 %) with 81.2 % yield of C 15 dicycloalkane under mild reaction conditions (190 °C, 4 MPa H 2 ). Controlled reactions of PC and probe molecules demonstrated the conversion of PC into C 15 dicycloalkanes involves PC depolymerization by direct cleavage of C-O bonds adjacent to benzene ring and ester group, forming C 15 aromatics and C 15 monophenols at the metal sites, followed by hydrogenation of C 15 aromatics rings on metallic Ni sites and HDO of C 15 monophenols on metal-acid dual sites parallel to generate C 15 dicycloalkane. The C-C cracking mainly occurred on the tertiary carbon adjacent to the benzene ring on acidic sites of HZSM-5, thus forming C 6 ∼C 9 monocyclic alkanes. The realization of this process can be attributed to the cooperation between metal sites and acid centers on Ni/HZSM-5. Besides, the metal-acid balance (MAB) in Ni/HZSM-5 significantly affected the HDO activity and product distribution. 20Ni/HZSM-5(200) with suitable MAB showed good HDO activity and excellent selectivity to C 15 dicycloalkane. In addition, the obtained catalyst was also capable of converting common real PC plastics wastes (CD disk, DVD disk and PC sheet) into cycloalkanes with the yield up to 98 % and exhibited excellent stability. This approach to construct inexpensive bifunctional catalysts highlights an efficient and reliable route for HDO of PC to sustainable aviation fuel, providing a new avenue towards a circular economy.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2023
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IF 2.2
Hongye Bai,Lihao Yu,Jinfu Xu,Xuliang Pang,Yajie Bai,Jianguo Cui,Weiqiang Fan
Decoration of metal-organic framework (MOF) has been considered as an effective route to improve the photoelectrochemical (PEC) performance of TiO 2 , but there is still a lack of understanding of the regulatory structure. Herein, Ni-MOF was rationally introduced by in-situ etching method, which helps for artificially regulating the coordination state of Ni sites. The photocurrent density (0.81 mA/cm 2 ) and IPCE value (33.1%) of TiO 2 -MOF-2 are about twice higher than that of pristine TiO 2 due to the rich unsaturated sites of Ni-MOF. Meanwhile, the saturated coordination has caused the decline of PEC performance because of the obvious steric hindrance . Therefore, this work presents an insight for the effect of coordination state on PEC activity especially in MOF system.
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ACS Catalysis
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2023
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IF 12.9
Dong Ji,Peng Guo,Yongjie Xi,Jinlei Li,Jia Wang,Tingting Wang,Fuwei Li
Selective tandem hydrogenation is a promising strategy for catalytic conversion of bulk raw materials with multifunctional groups into high-value-added chemicals via multiple-step reactions. Yet now, one of the current challenges is to develop a multifunctional and stable catalyst enabling the tandem catalysis rather than interrupting at any step reaction, particularly for supported nonprecious metal catalysts. In this work, we report tandem hydrogenation of bulk phthalic anhydride toward the one-pot synthesis of hexahydrophthalide, an emerging monomer of a recyclable polyester, over phosphorus-promoted Ni–Co bimetallic alloy nanoparticle catalysts. The surface composition of catalysts can be easily regulated by changing the Ni/Co molar ratio and the phosphorous functionalization strategy, which could then tune the product selectivity and enhance the stability of this tandem process. The optimal Ni3Co1@NC-P affords 88% selectivity for the desired product and demonstrates promising stability toward the tandem hydrogenation reaction. Systematic experimental and computational studies reveal that the adsorption strength of the intermediates and the ability of hydrogen activation can be altered by the formation of surface metallic Ni species, thus tuning the product selectivity. In addition, the oxidation resistance of Ni3Co1@NC-P was enhanced by the phosphorization treatment, which makes the bimetallic alloy successfully realize the tandem hydrogenation reaction. The finding of this work not only provides a convenient strategy to design and develop efficient and stable non-noble metal-based catalysts for selective tandem hydrogenation reactions, especially involving the hydrodeoxygenation reaction, but also fulfills the straightforward pathway for the preparation of degradable polyester monomer hexahydrophthalide.
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Arabian Journal of Chemistry
·
2023
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IF 6
Yongjun Shen,Yin Chen,Shuaikang Fang,Jae Kwang Park,Kun Feng
To solve the current energy and environmental dilemma, hydrogen energy is considered to be the best clean energy source to replace traditional fossil fuels. Water electrolysis as the main technology for hydrogen production has been affected by two half-reactions, making it difficult to improve the yield. To solve this problem, the development of inexpensive and efficient bifunctional electrocatalysts is the focus of current research. CuCo 2 S 4 /NF(Ni foam) nanowires are synthesized using a mild hydrothermal process and were later placed in a plasma reactor. Application of the voltage triggers a chemical reaction between the microdischarge wires and the sample. This leads to a change in the physical morphology of the catalyst and an improvement in its catalytic performance. The morphological characterization results show that the catalyst modification generates a distinct flower-like nanowire structure, which helps in the solid attachment of the catalyst to the nickel foam surface. The plasma-modified CuCo 2 S 4 /Ni foam (PA@CuCo 2 S 4 /NF) exhibits low overpotentials of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline solutions. Additionally, the Tafel slopes of the HER and OER are 85.9 mVdec −1 and 142.7 mVdec −1 , respectively, indicating optimal reaction kinetics. A cell voltage of only 1.55 V is required to provide a 10 mA cm −2 current during water splitting. This study validates the feasibility of using plasma technology to create high-performance electrocatalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Ningyi Chen,Shuang Wu,Bingjun Pan,Zhichao Yang,Bingcai Pan
Advanced techniques for nickel (Ni(II)) removal from polluted waters have long been desired but challenged by the diversity of Ni(II) species (most in the form of complexes) which could not be readily discriminated by the traditional analytical protocols. Herein, a colorimetric sensor array is developed to address the above issue based on the shift of the UV–vis spectra of gold nanoparticles (Au NPs) after interaction with Ni(II) species. The sensor array is composed of three Au NP receptors modified by N-acetyl-l-cysteine (NAC), tributylhexadecylphosphonium bromide (THPB), and the mixture of 3-mercapto-1-propanesulfonic acid and adenosine monophosphate (MPS/AMP), to exhibit possible coordination, electrostatic attraction, and hydrophobic interaction toward different Ni(II) species. Twelve classical Ni(II) species were selected as targets to systematically demonstrate the applicability of the sensor array under various conditions. Multiple interactions with Ni(II) species were evidenced to trigger the diverse Au NP aggregation behaviors and subsequently produce a distinct colorimetric response toward each Ni(II) species. With the assistance of multivariate analysis, the Ni(II) species, either as the sole compound or as mixtures, can be unambiguously discriminated with high selectivity in simulated and real water samples. Moreover, the sensor array is very sensitive with the detection limit in the range of 4.2 to 10.5 μM for the target Ni(II) species. Principal component analysis signifies that coordination dominates the response of the sensor array toward different Ni(II) species. The accurate Ni(II) speciation provided by the sensor array is believed to assist the rational design of specific protocols for water decontamination and to shed new light on the development of convenient discrimination methods for other toxic metals of concern.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xuan Liu,Jianying Wang,Zhongying Fang,Shuaiqi Gong,Dengke Xiong,Wei Chen,Deli Wu,Zuofeng Chen
Herein, an ultrafast electro-corrosion approach is developed for activating Ni foam (NF) into an efficient electrocatalyst for upcycling polybutylene terephthalate (PBT) waste plastic. The electro-corrosion process assisted by Cl − is completed by only 6 CV cycles (∼3 min) and the activity of the treated NF (T-NF), characterized by the integrated Ni 2+ /Ni 3+ peak area is enhanced by 150 times. The T-NF electrode exhibits excellent catalytic activity toward 1,4-butanediol oxidation , delivering a current density of 50 mA cm − 2 at 1.36 V (vs. RHE). This allows the electrocatalytic reforming of 1,4-butanediol component in PBT hydrolysate into succinate with a high Faraday efficiency 93%. The in-situ Raman and FTIR spectroscopies combining density functional theory calculations identify catalytically active centers, critical intermediates, and favorable pathway for 1,4-butanediol oxidation to succinate. This work provides an ultrafast one-step surface engineering strategy to turn pristine Ni foams into high-performance electrocatalysts for upcycling PBT plastic and other electrochemical applications.
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Inorganics
·
2023
·Vol. 11
·期 6
·236
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IF 2.9
Jia-Lin Cui,Zhong-Liang Liu,Hui-Hui Li,Chun-Zhong Li
The synthesis of highly efficient heterogeneous catalysts with uniformly dispersed noble metal particles and a suitable size is crucial for various industrial applications. However, the high cost and rarity of noble metals limit their economic efficiency, making it essential to improve the catalytic performance with lower noble metal loading. Herein, a two-step method was developed for the synthesis of uniformly dispersed ~3 nm Pt nanoparticles (NPs), strongly anchored on Ni(OH)2nanosheets (NSs), which was proven by adequate structural characterizations. XPS analysis demonstrated that Ni(OH)2NSs with abundant oxygen vacancies provided sufficient anchor sites for Pt NPs and prevented their agglomeration. The catalytic performance of Ptn/Ni(OH)2(n (represents the addition amount of Pt precursors during the synthesis, μmol) = 5, 10, 15, and 20) NSs with controllable Pt loading were evaluated via the reduction of 4-nitrophenol to 4-aminophenol as a model reaction. The Pt10/Ni(OH)2NSs exhibited the best activity and stability, with a reaction rate constant of 0.02358 s−1and negligible deterioration in ten reaction cycles. This novel synthetic method shows potentials for the synthesis of highly efficient noble-metal-supported catalysts for heterogeneous catalysis.Keywords:Pt/Ni(OH)2nanosheets;oxygen vacancy;heterogeneous catalysis;reduction of 4-nitrophenol
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International Journal of Electrochemical Science
·
2023
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IF 1.5
Li Zheng,Chao-Rui Zhang,Dan Zhao,Xuan Wanga,Ting-Ting Du
A β-Ni(OH) 2 flakes modified carbon paste electrode [Ni(OH) 2 /CPE] has fabricated for hydrazine sensing. The β-Ni(OH) 2 flakes derived from nickel hexacyanoferrate (NiHCF) through a facile in situ electrochemical method and characterized by Fourier transform infrared spectrometry, X-ray diffraction, and scanning electron microscopy. Meanwhile, the electrochemical performances of the modified electrode studied by electrochemical impedance spectroscopy, chronocoulometry, cyclic voltammetry, and linear sweep voltammetry. Owing to the large active surface area and enhanced electron transfer efficiency of β-Ni(OH) 2 flakes, the Ni(OH) 2 /CPE showed enhanced catalytic activity toward the oxidation of hydrazine compared with NiHCF/CPE and unmodified CPE. Under the optimized conditions, the amperometric current presented linear dependence on the concentration of hydrazine in the ranges of 0.1 ~ 600 μM with the detection limit of 0.04 μM. Furthermore, the sensor has applied for the determination of hydrazine in water samples.
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Nanomaterials
·
2023
·Vol. 13
·期 13
·1941
·
IF 5.3
Zhi Lu,Zhihao Zhou,Shilin Li,Gongliang Tan,Hangtian Chen,Zishuo Ge,Chong Chen,Guangxin Wang
Low-cost and high-performance electrocatalysts are crucial for water-splitting reactions. Some non-precious metal electrocatalysts are proved to be good replacements for noble metal due to the unique electronic structure features and excellent performance. In this work, binary Ni-Co-based layered double hydroxide nanoneedle arrays electrocatalysts are synthesized on Ni foam (NF) via a hydrothermal process. The microstructure and the catalytic performance of the catalyst changes significantly by regulating the molar ratio of Ni/Co. The theoretical analysis confirmed that the as-prepared NiCo-LDH nanoneedle arrays reveal a potential behavior in oxygen evolution reaction (OER) at a lower overpotential of 305 mV at 10.0 mA cm−2and a Tafel slope of 110.38 mV dec−1. The double-layer capacitance (Cdl) is 776 mF cm−2, which indicates that there are many active sites that are exposed on the surface for the electrocatalytic reaction. The results provide an obvious reference value to other types of LDH catalysts for the development of water electrolysis.Keywords:nanoneedle;Ni-Co based;electrolysis;OER;electrocatalyst
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ENERGY & FUELS
·
2023
·
IF 5.3
Yi Ren,Yujia Bai,Genxiang Wang,Yijian Liu,Chuancheng Mou,Jiayu Chen,Baohuan Wei,Hui Wang,Yuhan Sun
Efficient conversion of CO2 to value-added fuels or chemicals using electricity from renewable sources is an appealing approach to realize carbon neutrality. Under this background, it is crucial to design efficient and low-cost catalysts for CO2 electroreduction. Herein, we fabricated an electrocatalyst with the structure of Cu–Ni alloy nanoparticles grown on nitrogen-doped carbon nanotubes (CuxNi/NCNT, x = 2.4, 1, and 0.36) for electrochemical CO2 reduction reaction (CO2RR) via a hydrothermal method followed by pyrolysis. The optimized CuNi/NCNT demonstrates a favorable CO2RR performance with a CO Faradaic efficiency (FECO) of 94.8% and a current density of 26.6 mA cm–2 at −0.9 V versus the reversible hydrogen electrode (vs RHE) in the H-cell, far superior to those of single metal counterparts. Density functional theory (DFT) calculations unravel that the Cu–Ni alloys possess much lower free energy changes for the formation of the key COOH* intermediate than those of the Cu metal, thereby facilitating CO2 reduction into CO. Additionally, the CO2RR performance of CuNi/NCNT was further evaluated in the gas diffusion electrode (GDE) involved in the flow cell to examine the practical application of the prepared catalyst, which can deliver a current density of 124.6 mA cm–2 with a FECO of 92.8% at −1.1 V vs RHE. This work enriches electrocatalysts for highly efficient CO2 electroreduction to CO.
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Nanomaterials
·
2023
·Vol. 13
·期 6
·994
·
IF 5.3
Wei Dong,Qin Zhou,Wangqiang Shen,Le Yang,Peng Jin,Xing Lu,Yongfu Lian
Soot-containing terbium (Tb)-embedded fullerenes were prepared by evaporation of Tb4O7-doped graphite rods in an electric arc discharge chamber. After 1,2,4-trichlorobenzene extraction of the soot and rotary evaporation of the extract, a solid product was obtained and then dissolved into toluene by ultrasonication. Through a three-stage high-pressure liquid chromatographic (HPLC) process, Tb@C82(I, II) isomers were isolated from the toluene solution of fullerenes and metallofullerenes. With the success of the growth of cocrystals of Tb@C82(I, II) with Ni(OEP), the molecular structures of Tb@C82(I) and Tb@C82(II) were confirmed to be Tb@C2v(9)-C82and Tb@Cs(6)-C82, respectively, based on crystallographic data from X-ray single-crystal diffraction. Moreover, it was found that Tb@C82(I, II) isomers demonstrated different packing behaviors in their cocrystals with Ni(OEP). Tb@C2v(9)-C82forms a 1:1 cocrystal with Ni(OEP), in which Tb@C2v(9)-C82is aligned diagonally between the Ni(OEP) bilayers to form zigzag chains. In sharp contrast, Tb@Cs(6)-C82forms a 2:2 cocrystal with Ni(OEP), in which Tb@Cs(6)-C82forms a centrosymmetric dimer that is aligned linearly with Ni(OEP) pairs to form one-dimensional structures in the a–c lattice plane. In addition, the distance of a Ni atom in Ni(OEP) to the Cs(6)-C82cage is much shorter than that to the C2v(9)-C82one, indicative of a stronger π-π interaction between Ni(OEP) and the C82carbon cage in the cocrystal of Tb@CS(6)-C82and Ni(OEP). Density functional theory calculations reveal that the regionally selective dimerization of Tb@CS(6)-C82is the result of a dominant unpaired spin existing on a particular C atom of the CS(6)-C82cage.Keywords:metallofullerene;terbium;cocrystals;centrosymmetric dimer;unpaired spin
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