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In-situ tracking CO_(2)-assisted isothermal-isobaric synthesis of selfassembled Bi-based photocatalyst using novel SAXS/XRD/XAFS combined technique
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作者 Yunpeng Liu Shunzheng Zhao +7 位作者 Jiajun Zhong Jianglong Liu baotong chen You Liao Lei Yao Zhongjun chen Buxing Han Zhonghua Wu 《Science China Materials》 SCIE EI CAS CSCD 2024年第11期3609-3621,共13页
The synthetic path of a catalyst determines its morphology,species,and performance,and in-situ monitoring the catalyst formation process is fascinating and challenging.Herein,a newly developed synchrotron radiation sm... The synthetic path of a catalyst determines its morphology,species,and performance,and in-situ monitoring the catalyst formation process is fascinating and challenging.Herein,a newly developed synchrotron radiation smallangle X-ray scattering/X-ray diffraction/X-ray absorption fine structure(SAXS/XRD/XAFS)combined technique was used to in-situ monitor the isothermal-isobaric synthesis process of CO_(2)-assisted(BiO)_(2)CO_(3)(BOC)photocatalyst,and the atomic near-neighbor structure,crystalline structure and nanoscale particle size evolution with reaction time were simultaneously captured.The results show that both polyvinyl pyrrolidone and CO_(2)formed uniformly-distributed nano-sized scatterers in the Bi-based precursor solution,presenting short-range ordered structures to a certain extent.The as-prepared BOC catalytic particles underwent the evolution process of initial Bi(OH)3 precipitate,early-stage formed KBiO_(2)molecules,intermediate amorphous(BiO)4CO3(OH)2 nanoparticles,and finally crystallized flower-like BOC particles self-assembled by nanosheets.The flower-like BOC particles,Bi/BOC composite,and Bi nanospheres were further prepared with different synthesis paths.Flower-like BOC particles showed the best photocatalytic degradation performance of RhB.Scavenger experiment and theoretical calculation revealed the photocatalytic mechanisms of BOC.This work has implications for path-dependent synthesis of other catalysts. 展开更多
关键词 SAXS/XRD/XAFS combined technique (BiO)_(2)CO_(3) in-situ tracking formation process photodegradation
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Interfacial engineering of SnO_(2)/Bi_(2)O_(2)CO_(3)heterojunction on heteroatoms-doped carbon for high-performance CO_(2)electroreduction to formate 被引量:2
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作者 Danni Wang Tingting Sun +8 位作者 Lianbin Xu Lei Gong baotong chen Pianpian Zhang Tianyu Zheng Qingmei Xu Houhe Pan Yuexing Zhang Jianzhuang Jiang 《Nano Research》 SCIE EI CSCD 2023年第2期2278-2285,共8页
Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust cata... Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust catalysts through interface engineering is significant for electrocatalytic CO_(2)reduction(ECR)but remains a grand challenge.Herein,SnO2/Bi_(2)O_(2)CO_(3)heterojunction on N,S-codoped-carbon(SnO_(2)/BOC@NSC)with efficient ECR performance was firstly constructed by a facile synthetic strategy.When the SnO_(2)/BOC@NSC was utilized in ECR,it exhibits a large formic acid(HCOOH)partial current density(JHCOOH)of 86.7 mA·cm^(−2)at−1.2 V versus reversible hydrogen electrode(RHE)and maximum Faradaic efficiency(FE)of HCOOH(90.75%at−1.2 V versus RHE),respectively.Notably,the FEHCOOH of SnO_(2)/BOC@NSC is higher than 90%in the flow cell and the JHCOOH of SnO_(2)/BOC@NSC can achieve 200 mA·cm^(−2)at−0.8 V versus RHE to meet the requirements of industrialization level.The comparative experimental analysis and in-situ X-ray absorption fine structure reveal that the excellent ECR performance can be ascribed to the synergistic effect of SnO_(2)/BOC heterojunction,which enhances the activation of CO_(2)molecules and improves electron transfer.This work provides an efficient SnO_(2)-based heterojunction catalyst for effective formate production and offers a novel approach for the construction of new types of metal oxide heterostructures for other catalytic applications. 展开更多
关键词 HETEROJUNCTION charge transfer electrochemical CO_(2)reduction flow cell in-situ X-ray absorption fine structure
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Metalphthalocyanine frameworks grown on TiO_(2)nanotubes for synergistically and efficiently electrocatalyzing urea production from CO_(2)and nitrate 被引量:2
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作者 Ning Li Hui Gao +8 位作者 Zhixin Liu Qianjun Zhi Bowen Li Lei Gong baotong chen Tao Yang Kang Wang Peng Jin Jianzhuang Jiang 《Science China Chemistry》 SCIE EI CAS CSCD 2023年第5期1417-1424,共8页
Electrocatalytic synthesis of urea from CO_(2)and NO_(3)^(-)under ambient conditions provides an appealing alternative to the traditional energy-intensive urea synthetic protocol.Highly active and selective electrocat... Electrocatalytic synthesis of urea from CO_(2)and NO_(3)^(-)under ambient conditions provides an appealing alternative to the traditional energy-intensive urea synthetic protocol.Highly active and selective electrocatalysts for efficient urea production are therefore urgently desired owing to the unsatisfactory performance of the thus far reported catalysts.Herein,a phthalocyaninebased(Pc-based)covalent organic framework(COF),namely Co Pc-COF,fabricated from the nucleophilic substitution reaction of hexadecafluorophthalocyaninato cobalt with octahydroxylphthalocyanine cobalt,in situ grew on the surface of multilayered Ti O_(2)nanotubes(NTs),generating the Co Pc-COF@Ti O_(2)NTs composite.Powder X-ray diffraction analysis in combination with electron microscopy measurements discloses the uniform coating of crystalline Co Pc-COF on the multilayered Ti O_(2)NTs in Co Pc-COF@Ti O_(2)NTs.Remarkably,electrochemical tests reveal the superior electrocatalytic activity of Co Pc-COF@Ti O_(2)NTs towards urea production from CO_(2)and NO3-with a record-high yield of 1,205μg h^(-1)cm^(-2)and an outstanding Faraday efficiency of 49%at-0.6 V versus reversible hydrogen electrode due to the significant synergistic catalysis effect.In situ attenuated total reflection infrared spectroscopic investigation and theoretical calculations unveil the efficient C–N coupling reaction between*CO intermediate derived from CO_(2)on Co Pc moieties and*NH2intermediate formed from NO_(3)^(-)on Ti O_(2)NTs during the urea formation process over Co Pc-COF@Ti O_(2)NTs.This work should be helpful towards designing and fabricating high-performance electrocatalysts for sustainable synthesis of urea through efficient synergistic effect of multiactive centers. 展开更多
关键词 covalent organic frameworks PHTHALOCYANINE TiO_(2) electrocatalytic urea synthesis C–N bond coupling
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