ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xue Zhao,Ziqiong Yang,Artem V. Kuklin,Glib V. Baryshnikov,Hans Ågren,Xiaohai Zhou,Haibo Zhang
Currently, the development of stable electrochemical nitrogen reduction reaction (ENRR) catalysts with high N2 conversion activity and low cost to instead of the traditional Haber-Bosch ammonia production process of high-energy consumption remains a great challenge for researchers. Here, we have immobilized reductive closo-[B12H11]− boron clusters on a carbon nanotubes (CNT) surface and have successfully prepared a novel Au-CNT catalyst with extraordinary ENRR activity after adding HAuCl4 to the CNT-[B12H11]− precursor. The excellent properties of ammonia yield (57.7 μg h–1 cm–2) and Faradaic efficiency (11.97%) make it possible to achieve using this Au-CNT catalyst in large-scale industrial production of ammonia. Furthermore, its outstanding cyclic stability and long-term tolerability performance make it one of the most cost-effective catalysts to date. Here, by means of density functional theory we disclose the associative mechanism of N2-to-NH3 conversion on the Au(111) surface, providing visual theoretical support for the experimental results.
研究领域:
材料科学
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化学工程
·
理论化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Yuwen Wang,Zenghui Bi,Xue Zhao,Abdukader Abdukayum,Shuxing Zhou,Haibo Zhang,Jianbing Chen,Fang Tan,Anran Chen,Thomas Wågberg,Guangzhi Hu
The reduction of nitroaromatics to aminoaromatics is essential for fine chemical production and effective sewage treatment. However, the activity of an external catalyst is essential for the reaction. In this study, Pd nanocrystals were anchored in situ on two-dimensional graphene oxide (GO), which acted as a catalyst support with high specific surface area. The oxygen-containing groups on the surface of GO bonded to the functionally rich boron clusters through hydrogen bonding interactions. A mildly reducible closed-dodecahydrododecaboric acid anion cluster ( closo‑ [B 12 H 12 ] 2– ) was employed as the target site. The mild reducibility of closo‑ [B 12 H 12 ] 2– resulted in a wide dispersion of ultrafine Pd nanocrystals on GO. Under ambient conditions, Pd/BGO rapidly hydrogenated nitroaromatics, such as 4-nitrophenol, to aminoaromatics with approximately 100% efficiency. Moreover, Pd/BGO retained its high catalytic activity for the hydrogenation/reduction of 4-nitrophenol after five catalytic cycles. Therefore, Pd/BGO could be a promising and economically viable candidate for various practical applications. The proposed innovative preparation strategy and highly efficient catalytic activity suggested the effective performance of closo‑ [B 12 H 12 ] 2– as nanometal nucleation target sites. In addition to providing an alternate route for preparing supported nanometals, this study presents a stable and efficient catalyst for the hydrogenation of nitroaromatics.
研究领域:
化学工程
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材料科学
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催化技术
✓ 已验证
DOI
高影响因子
INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
An-Na Chen,Lei Liu,Chun-Yang Pan
Three copper complex borates, [Cu(en) 2 ]·[B 4 O 5 (OH) 4 ]·2H 3 BO 3 ( 1 , en = ethylenediamine), [Cu(Eten) 2 ]·[B 5 O 6 (OH) 4 ] 2 ( 2 , Eten = N -ethyl ethylenediamine) and [Cu(Dmen) 2 ]·[B 10 O 13 (OH) 6 ] ( 3, Dmen = N,N -dimethyl ethylenediamine) have been successfully synthesized and structurally characterized by single-crystal X-ray diffraction, PXRD, and FTIR. Their oxoboron clusters are [B 4 O 5 (OH) 4 ] 2− , [B 5 O 6 (OH) 4 ] − and [B 10 O 13 (OH) 6 ] 2− , respectively. Copper ion was used as the central atom, ethylenediamine and its derivatives were selected as ligand. The structure of oxoboron clusters in 1 , 2 and 3 can be modulated through varying ethylenediamine derivative ligand, as well as temperature and pressure of reaction system. These copper complex borates exhibited open framework formed by the interconnection of hydrogen bonds of oxoboron clusters. Moreover, the oxygen reduction reaction activity of these borate-based catalysts was investigated. The half-wave potential values of the products after heating 1 – 3 with carbon at 600 °C (1/C-600, 2/C-600 and 3/C-600) were 0.817, 0.80 and 0.73 V, respectively.
研究领域:
材料化学
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电催化
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配位化学
✓ 已验证
产品关联
DOI
高影响因子
ChemNanoMat
·
2019
·Vol. 5
·期 9
·1209-1215
·
IF 3.431
Bin Qi,Chenchen Wu,Jun Liu,Haibo Zhang
Graphical On the assembly line : A supramolecular self-assembly strategy was successfully applied to prepare magnetic Pd nanocomposites with excellent catalytic performance. Supramolecular chaotropic effect is a new topic in the field of nanocomposites (NCs) fabrication. Herein, this strategy was applied to prepare magnetic Fe 3 O 4 @γ-CD-boron cluster (SSAs)@Pd NCs in situ via a facile two-step process, involving a supramolecular assembly process on Fe 3 O 4 NPs and in situ formation of Pd nanoparticles. Boron clusters ([ closo -B 12 H 12 ] 2− ) played a dual role in this synthetic process, and were used as a superchaotropic anion to interact with γ-CD to form supramolecular self-assemblies (SSAs), as well as efficient reductant to in situ reduce Pd(II) to Pd(0). Ascribed to the electrostatic attraction of boron clusters and capping effect of γ-CD, ultrafine Pd nanoparticles were successfully coated on the Fe 3 O 4 @SSAs composites to fabricate Fe 3 O 4 @SSAs@Pd NCs. A combination of UV spectra, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, X-ray diffraction, and energy dispersive X-ray spectroscopy was used to verify the formation of these magnetic Pd NCs. The ultrafine metallic Pd NPs imparted the magnetic composites with great potential in catalysis, especially for Suzuki coupling reactions. Remarkably, the obtained Fe 3 O 4 @SSAs@Pd NCs showed good catalytic performance, high stability and easy recycling via an external magnet.
研究领域:
材料科学
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催化化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Bin Gao,Bin Qiu,Mingji Zheng,Zhankai Liu,Wen-Duo Lu,Qiang Wang,Jun Xu,Feng Deng,An-Hui Lu
Boron-containing zeolites have been demonstrated as active catalysts for oxidative dehydrogenation of propane (ODHP) to propene. The challenge is that the origin of the boron active sites remains an unsolved issue. In this study, self-pillared boron-containing MFI zeolite nanosheets with an ultrathin b-axis were synthesized, which exhibited low-temperature activity and stability in the ODHP process. A combination of in situ diffuse reflectance infrared Fourier transform, two-dimensional 11B multiple-quantum MAS NMR, and 11B{1H} dipolar-heteronuclear multiple-quantum correlation NMR measurements revealed that the MFI zeolite nanosheets with the characteristics of a high specific surface area and abundant Si–OH groups allowed dynamic self-dispersion of highly mobile boron clusters through condensation with surrounding Si–OH groups. The increased number of stable and dispersed oligomeric boron species was responsible for the enhanced catalytic performance and stability in the ODHP process. The catalysts were active at a temperature as low as 390 °C. Upon raising the temperature to 430 °C, a propane conversion of 14.1% could be achieved together with a selectivity of 80.1% toward all olefins.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
POLYHEDRON
·
2024
·
IF 2.4
An-Na Chen,Yan-Ling Deng,Chun-Yang Pan
Two imidazole-based ligand-nickel borates, [Ni(1-ipIM) 3 ·B 6 O 7 (OH) 6 ]·[H 3 BO 3 ]·2·.5H 2 O ( 1 , 1-ipIM = 1-isopropylimidazole) and [Ni(1-pIM) 6 ]·[B 5 O 6 (OH) 4 ]·2H 2 O ( 2 , 1-pIM = 1-propylimidazole) have been synthesized and structurally characterized by single-crystal X-ray diffraction, PXRD, FTIR. The oxoboron cluster structures of 1 and 2 were modulated through changing the carbon-branched structure on the N -site of the imidazole-based ligand using metallic nickel as the central atom. It is noteworthy that the structure of 1 is a hybridized skeleton formed by N -Ni-O-B bonds. The electrocatalytic oxygen reduction reaction (ORR) activity of these borate-based catalysts was investigated. The half-wave potential ( E 1/2 ) values of 1 -based and 2 -based were about 0.825 and 0.80 V, respectively.
研究领域:
无机化学
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电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Rui Bai,Yuelong Liu,Yicheng Zhang,Yingtang Zhou,Haibo Zhang,Yan Zhao,Xue Zhao
To promote the greening and economization of industrial production, the development of advanced catalyst manufacturing technology with high activity and low cost is an indispensable part. In this study, nitrogen-doped hollow carbon spheres (NHCSs) were used as anchors to construct a supramolecular coating formed by the self-assembly of boron clusters and β -cyclodextrin by surface crystallization strategy, with the help of the weak reducing agent characteristics of boron clusters, highly dispersed ultra-small nano-palladium particles were in-situ embedded on the surface of NHCSs. The deoxygenation hydrogenation of nitroaromatics and the reduction of nitrate to ammonia were used as the representatives of thermal catalytic reduction and electrocatalytic reduction respectively. The excellent properties of the constructed Pd/NHCSs were proved by the probe reaction. In the catalytic hydrogenation of nitroaromatics to aminoaromatics, the reaction kinetic rate and activation energy are at the leading level. At the same time, the constructed Pd/NHCSs can also electrocatalytically reduce nitrate to high value-added ammonia with high activity and selectivity, and the behavior of Pd/NHCSs high selectivity driving nitrate conversion was revealed by density functional theory and in situ attenuated total reflection Fourier transform infrared (ATRFTIR) technique. These results all reflect the feasibility and superiority of in-situ anchoring ultra-small nano-metals as catalysts by surface crystallization to build a supramolecular cladding with reducing properties, which is an effective way to construct high-activity and low-cost advanced catalysts.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）