The electrochemical CO_(2)reduction(ECR)to hydrocarbon products is an attractive pathway to decrease CO_(2)emission and advance a carbon-neutral process.Among the products of ECR,methane(CH_(4))stands out due to its h...The electrochemical CO_(2)reduction(ECR)to hydrocarbon products is an attractive pathway to decrease CO_(2)emission and advance a carbon-neutral process.Among the products of ECR,methane(CH_(4))stands out due to its high calorific value,serving as the main component of natural gas.However,the development of ECR catalysts capable of producing CH_(4)with both high activity and stability remains critically urgent.This review summarizes and explores the research progress and future application strategies for ECR toward CH_(4)production.Combining experiments,in-situ characterizations,and theoretical calculations,this review examines mechanism of CH_(4)formation in ECR.It then clarifies key factors affecting Cu-based catalysts for CH_(4)production,including facet dependence,size effects,and valence states.Next,this review details emerging strategies such as sub-nanoscale catalysts,Cu/oxides interface engineering,and Cu surface modification.Finally,future directions highlight in-situ characterization,reactor design,and high-throughput screening,guiding industrial CH_(4)production.展开更多
Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of phot...Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm^(-2) and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.展开更多
The crystal of binuclear zinc complex Zn2(dhaash)2(py)4 was obtained in DMF and pyridine, where H2dhaash is 2,4-dihydroxy-5-acetylacetophenone-N-salicylhydrazone. It has been characterized by IR, UV, element analysis ...The crystal of binuclear zinc complex Zn2(dhaash)2(py)4 was obtained in DMF and pyridine, where H2dhaash is 2,4-dihydroxy-5-acetylacetophenone-N-salicylhydrazone. It has been characterized by IR, UV, element analysis and X-ray single crystal diffraction. The crystallographic data were as follows: monoclinic system, space group P21 / c, a=1.108 98(11) nm, b=1.640 84(16) nm, c=1.445 14(14) nm, β=108.617(2)°, Z=2, V=2.492 1(4) nm3, Dc=1.466 g·cm-3, Mr=1 099.74, μ=1.031 mm-1, F(000)=1 136 and the final R=0.044 8 and wR=0.105 8 for 4 143 observed reflections with I≥2σ(I), respectively. The X-ray crystal structure analysis revealed that, in the centrosymmetric binuclear complex molecule, two zinc髤 centers are linked by two oxygen atoms (O(3) and O(3A)), respectively. Zn(1)...Zn(1A) distance is 0.314 81(6) nm, O(3)...O(3A) distance is 0.270 4(2) nm. Every zinc髤 ion has an elongated octahedral coordination. For example, the two pyridine nitrogen atoms, one oxygen atom and one nitrogen atom from salicylhydrazone, one oxygen atom from 2,4-dihydroxy-5-acetylacetophenone in one dhaash2- ligand and one oxygen atom from 2,4-dihydroxy-5-acetylacetophenone in another dhaash2- ligand coordinated to zinc髤 ion, respectively. Two zinc髤 ions and all the 72 non-hydrogen atoms in the two dhaash2- ligands are in the same plane. CCDC: 261929.展开更多
The title cluster compound [WS4Cu3Br(bipy)2] has been synthesized by the reaction of (NH4)2, CuBr and 2,2′ bipy in DMF solution. Single crystal X ray diffraction data show that the compound has a nest shaped structur...The title cluster compound [WS4Cu3Br(bipy)2] has been synthesized by the reaction of (NH4)2, CuBr and 2,2′ bipy in DMF solution. Single crystal X ray diffraction data show that the compound has a nest shaped structure. Nonlinear optical properties (NLO) of the cluster were investigated by a Z scan technique with a pulsed laser at 532nm. The cluster exhibits the strong NLO absorption and a self defocusing effect (effective non linear absorption coefficient, α2eff=7.3×10-11mW-1; effective non linear refractive index, n2eff=3.9×10-11esu) when measured in a 6.0×10-4mol·dm-3 DMF solution. CCDC: 200397.展开更多
The reaction of N-n-Bu4MnO4 with Mn(Oac) 2 · 4H2O and butenoic acid in nonaqueous solvents leads to the formation of the complex [Mn3O(O2CCH = CHCH3) 6(py) 3] ClO4 · py (1). The crystal structure was determi...The reaction of N-n-Bu4MnO4 with Mn(Oac) 2 · 4H2O and butenoic acid in nonaqueous solvents leads to the formation of the complex [Mn3O(O2CCH = CHCH3) 6(py) 3] ClO4 · py (1). The crystal structure was determined.The complex crystallizes in hexagonal, space group P63/m, unit cell parameters, a = 1. 2456(1)nm, b = 1. 2456(1) nm, c = 1. 8741(1) nm, V=2. 5181(3) nm3, Z =2, and final R1 =0. 0565, wR2 =0. 1465. Variable tem-perature solid tate magnetic susceptibility study shows that the complex [Mn3O(O2CCH = CHCH3)6(py)3] ClO4 (2) has an antiferromagnetic exchange interaction.展开更多
V（HSO4）3 has been found to be an efficient reagent for the promotion of the oxidation of alcohols and trimethylsilyl, tetrahydropyranyl and methoxymethyl ethers to their corresponding carbonyl compounds with Cu（NO3...V（HSO4）3 has been found to be an efficient reagent for the promotion of the oxidation of alcohols and trimethylsilyl, tetrahydropyranyl and methoxymethyl ethers to their corresponding carbonyl compounds with Cu（NO3）2-3H2O in the absence of solvent.展开更多
A new emissive mononuclear homoleptic Cu（Ⅰ） complex of 5-rert-butyl-3-（6-methyl-2-pyridyl）-1H-1,2,4-triazole（bmptzH）,[Cu（bmptzH）2]（ClO4）（1）,has been synthesized by treatment of[Cu（PPh_3）2（CH3CN）2]（C...A new emissive mononuclear homoleptic Cu（Ⅰ） complex of 5-rert-butyl-3-（6-methyl-2-pyridyl）-1H-1,2,4-triazole（bmptzH）,[Cu（bmptzH）2]（ClO4）（1）,has been synthesized by treatment of[Cu（PPh_3）2（CH3CN）2]（ClO4） or [Cu（CH3CN）4]（ClO4） with the bmptzH ligand.It is revealed that complex 1 displays a distorted N4 tetrahedral arrangement formed by two bmptzH chelates,in which bmptzH adopts a neutral bidentate chelating coordination mode using the N atom of the pyridyl ring and the 4-N not 2-N atom of the 1,2,4-triazolyl ring.It is shown that complex 1 is highly stable and exhibits good luminescence properties in solution and solid states at room temperature due to the introduction of a methyl group at the ortho-position of the pyridyl ring.展开更多
文摘The electrochemical CO_(2)reduction(ECR)to hydrocarbon products is an attractive pathway to decrease CO_(2)emission and advance a carbon-neutral process.Among the products of ECR,methane(CH_(4))stands out due to its high calorific value,serving as the main component of natural gas.However,the development of ECR catalysts capable of producing CH_(4)with both high activity and stability remains critically urgent.This review summarizes and explores the research progress and future application strategies for ECR toward CH_(4)production.Combining experiments,in-situ characterizations,and theoretical calculations,this review examines mechanism of CH_(4)formation in ECR.It then clarifies key factors affecting Cu-based catalysts for CH_(4)production,including facet dependence,size effects,and valence states.Next,this review details emerging strategies such as sub-nanoscale catalysts,Cu/oxides interface engineering,and Cu surface modification.Finally,future directions highlight in-situ characterization,reactor design,and high-throughput screening,guiding industrial CH_(4)production.
文摘Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm^(-2) and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.
文摘The crystal of binuclear zinc complex Zn2(dhaash)2(py)4 was obtained in DMF and pyridine, where H2dhaash is 2,4-dihydroxy-5-acetylacetophenone-N-salicylhydrazone. It has been characterized by IR, UV, element analysis and X-ray single crystal diffraction. The crystallographic data were as follows: monoclinic system, space group P21 / c, a=1.108 98(11) nm, b=1.640 84(16) nm, c=1.445 14(14) nm, β=108.617(2)°, Z=2, V=2.492 1(4) nm3, Dc=1.466 g·cm-3, Mr=1 099.74, μ=1.031 mm-1, F(000)=1 136 and the final R=0.044 8 and wR=0.105 8 for 4 143 observed reflections with I≥2σ(I), respectively. The X-ray crystal structure analysis revealed that, in the centrosymmetric binuclear complex molecule, two zinc髤 centers are linked by two oxygen atoms (O(3) and O(3A)), respectively. Zn(1)...Zn(1A) distance is 0.314 81(6) nm, O(3)...O(3A) distance is 0.270 4(2) nm. Every zinc髤 ion has an elongated octahedral coordination. For example, the two pyridine nitrogen atoms, one oxygen atom and one nitrogen atom from salicylhydrazone, one oxygen atom from 2,4-dihydroxy-5-acetylacetophenone in one dhaash2- ligand and one oxygen atom from 2,4-dihydroxy-5-acetylacetophenone in another dhaash2- ligand coordinated to zinc髤 ion, respectively. Two zinc髤 ions and all the 72 non-hydrogen atoms in the two dhaash2- ligands are in the same plane. CCDC: 261929.
文摘The title cluster compound [WS4Cu3Br(bipy)2] has been synthesized by the reaction of (NH4)2, CuBr and 2,2′ bipy in DMF solution. Single crystal X ray diffraction data show that the compound has a nest shaped structure. Nonlinear optical properties (NLO) of the cluster were investigated by a Z scan technique with a pulsed laser at 532nm. The cluster exhibits the strong NLO absorption and a self defocusing effect (effective non linear absorption coefficient, α2eff=7.3×10-11mW-1; effective non linear refractive index, n2eff=3.9×10-11esu) when measured in a 6.0×10-4mol·dm-3 DMF solution. CCDC: 200397.
文摘The reaction of N-n-Bu4MnO4 with Mn(Oac) 2 · 4H2O and butenoic acid in nonaqueous solvents leads to the formation of the complex [Mn3O(O2CCH = CHCH3) 6(py) 3] ClO4 · py (1). The crystal structure was determined.The complex crystallizes in hexagonal, space group P63/m, unit cell parameters, a = 1. 2456(1)nm, b = 1. 2456(1) nm, c = 1. 8741(1) nm, V=2. 5181(3) nm3, Z =2, and final R1 =0. 0565, wR2 =0. 1465. Variable tem-perature solid tate magnetic susceptibility study shows that the complex [Mn3O(O2CCH = CHCH3)6(py)3] ClO4 (2) has an antiferromagnetic exchange interaction.
基金the University of Guilan Research Council for the partial support of this work
文摘V（HSO4）3 has been found to be an efficient reagent for the promotion of the oxidation of alcohols and trimethylsilyl, tetrahydropyranyl and methoxymethyl ethers to their corresponding carbonyl compounds with Cu（NO3）2-3H2O in the absence of solvent.
基金supported by the National Natural Science Foundation of China(Nos.21561013,21501077)the Major Program of Jiangxi Provincial Natural Science Foundation of China for Young Scholar(Nos.20143ACB21017,20161ACB21013)+1 种基金the Jiangxi Provincial Natural Science Foundation of China(Nos.20142BAB203001,20151BAB213003)the Program for Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology
文摘A new emissive mononuclear homoleptic Cu（Ⅰ） complex of 5-rert-butyl-3-（6-methyl-2-pyridyl）-1H-1,2,4-triazole（bmptzH）,[Cu（bmptzH）2]（ClO4）（1）,has been synthesized by treatment of[Cu（PPh_3）2（CH3CN）2]（ClO4） or [Cu（CH3CN）4]（ClO4） with the bmptzH ligand.It is revealed that complex 1 displays a distorted N4 tetrahedral arrangement formed by two bmptzH chelates,in which bmptzH adopts a neutral bidentate chelating coordination mode using the N atom of the pyridyl ring and the 4-N not 2-N atom of the 1,2,4-triazolyl ring.It is shown that complex 1 is highly stable and exhibits good luminescence properties in solution and solid states at room temperature due to the introduction of a methyl group at the ortho-position of the pyridyl ring.
