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Check Digit Verification of cas no

The CAS Registry Mumber 1641-69-6 includes 7 digits separated into 3 groups by hyphens. The first part of the number,starting from the left, has 4 digits, 1,6,4 and 1 respectively; the second part has 2 digits, 6 and 9 respectively.
Calculate Digit Verification of CAS Registry Number 1641-69:
(6*1)+(5*6)+(4*4)+(3*1)+(2*6)+(1*9)=76
76 % 10 = 6
So 1641-69-6 is a valid CAS Registry Number.

1641-69-6SDS

SAFETY DATA SHEETS

According to Globally Harmonized System of Classification and Labelling of Chemicals (GHS) - Sixth revised edition

Version: 1.0

Creation Date: Aug 19, 2017

Revision Date: Aug 19, 2017

1.Identification

1.1 GHS Product identifier

Product name methylidyneoxidanium

1.2 Other means of identification

Product number -
Other names Carbon-13C monoxide

1.3 Recommended use of the chemical and restrictions on use

Identified uses For industry use only.
Uses advised against no data available

1.4 Supplier's details

1.5 Emergency phone number

Emergency phone number -
Service hours Monday to Friday, 9am-5pm (Standard time zone: UTC/GMT +8 hours).

More Details:1641-69-6 SDS

1641-69-6Relevant articles and documents

Efficient and Selective CO2 Reduction Integrated with Organic Synthesis by Solar Energy

Guo, Qing,Liang, Fei,Li, Xu-Bing,Gao, Yu-Ji,Huang, Mao-Yong,Wang, Yang,Xia, Shu-Guang,Gao, Xiao-Ya,Gan, Qi-Chao,Lin, Zhe-Shuai,Tung, Chen-Ho,Wu, Li-Zhu

, p. 2605 - 2616 (2019)

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Engineering a CsPbBr3-based nanocomposite for efficient photocatalytic CO2 reduction: Improved charge separation concomitant with increased activity sites

Guo, Xiao-Xuan,Tang, Shang-Feng,Mu, Yan-Fei,Wu, Li-Yuan,Dong, Guang-Xing,Zhang, Min

, p. 34342 - 34348 (2019)

Metal-halide perovskite nanocrystals have emerged as one of the promising photocatalysts in the photocatalysis field owing to their low-cost and excellent optoelectronic properties. However, this type of nanocrystals generally displays low activity in photocatalytic CO2 reduction owing to the lack of intrinsic catalytic sites and insufficient charge separation. Herein, we functionalized CsPbBr3 nanocrystals with graphitic carbon nitride, containing titanium-oxide species (TiO-CN) to develop an efficient composite catalyst system for photocatalytic CO2 reduction using water as the electron source. Compared to its congener with pristine CsPbBr3, the introduction of TiO-CN could not only increase the number of active sites, but also led to a swift interfacial charge separation between CsPbBr3 and TiO-CN due to their favorable energy-offsets and strong chemical bonding behaviors, which endowed this composite system with an obviously enhanced photocatalytic activity in the reduction of CO2 to CO with water as the sacrificial reductant. Over 3-fold and 6-fold higher activities than those of pristine CsPbBr3 nanocrystals and TiO-CN nanosheets, respectively, were observed under visible light irradiation. Our study provides an effective strategy for improving the photocatalytic activity of metal-halide perovskite nanocrystals, thus promoting their photocatalytic application in the field of artificial photosynthesis.

A porous hybrid material based on calixarene dye and TiO2 demonstrating high and stable photocatalytic performance

Chen, Yi-Fan,Huang, Jian-Feng,Shen, Min-Hui,Liu, Jun-Min,Huang, Li-Bo,Zhong, Yu-Hui,Qin, Su,Guo, Jing,Su, Cheng-Yong

, p. 19852 - 19861 (2019)

A highly robust hybrid material based on calixarene dye (HO-TPA) and titanium dioxide with a micro/mesoporous structure and a large surface area (denoted as HO-TPA-TiO2) has been prepared by a facile sol-gel method. When Pt nanoparticles (Pt NP

Constructed Z-Scheme g-C3N4/Ag3VO4/rGO Photocatalysts with Multi-interfacial Electron-Transfer Paths for High Photoreduction of CO2

Gao, Ming,Sun, Linlin,Ma, Changchang,Li, Xin,Jiang, Haopeng,Shen, Dong,Wang, Huiqin,Huo, Pengwei

, p. 1755 - 1766 (2021)

Z-scheme g-C3N4/Ag3VO4/reduced graphene oxide (rGO) photocatalysts with multi-interfacial electron-transfer paths enhancing CO2 photoreduction under UV-vis light irradiation were successfully prepared by a hydrothermal process. Transmission electron microscope images displayed that the prepared photocatalysts have a unique 2D-0D-2D ternary sandwich structure. Photoelectrochemical characterizations including TPR, electrochemical impedance spectroscopy, photoluminescence, and linear sweep voltammetry explained that the multi-interfacial structure effectively improved the separation and transmission capabilities of photogenerated carriers. Electron spin resonance spectroscopy and band position analysis proved that the electron-transfer mode of g-C3N4/Ag3VO4 meets the Z-scheme mechanism. The introduction of rGO provided more electron-transfer paths for the photocatalysts and enhanced the stability of Ag-based semiconductors. In addition, the π-πconjugation effect between g-C3N4 and rGO further improved the generation and separation efficiency of photogenerated electron-hole pairs. Then, the multiple channels (Ag3VO4 → CN, Ag3VO4 → rGO → CN, and rGO → CN) due to the 2D-0D-2D structure greatly improving the photocatalytic CO2 reduction ability have been discussed in detail.

Activity and selectivity regulation through varying the size of cobalt active sites in photocatalytic CO2 reduction

Mu, Qiaoqiao,Zhu, Wei,Yan, Gangbin,Lian, Yuebin,Yao, Yuanzhou,Li, Qin,Tian, Yuyu,Zhang, Peng,Deng, Zhao,Peng, Yang

, p. 21110 - 21119 (2018)

The development of efficient and economical catalysts for photocatalytic reduction of CO2 into chemical feedstocks is highly desirable for addressing both the global energy crisis and carbon emission problem. Herein, a series of carbonized coba

Photoelectrochemical CO2Reduction by a Molecular Cobalt(II) Catalyst on Planar and Nanostructured Si Surfaces

He, Da,Jin, Tong,Li, Wei,Pantovich, Sebastian,Wang, Dunwei,Li, Gonghu

, p. 13064 - 13067 (2016)

In the presence of a molecular CoIIcatalyst, CO2reduction occurred at much less negative potentials on Si photoelectrodes than on an Au electrode. The addition of 1 % H2O significantly improved the performance of the CoIIcatalyst. Photovoltages of 580 and 320 mV were obtained on Si nanowires and a planar Si photoelectrode, respectively. This difference likely originated from the fact that the multifaceted Si nanowires are better in light harvesting and charge transfer than the planar Si surface.

Pulse-response TAP studies of the reverse water-gas shift reaction over a Pt/CeO2 catalyst

Goguet,Shekhtman,Burch,Hardacre,Meunier,Yablonsky

, p. 102 - 110 (2006)

The temporal analysis of products (TAP) technique was successfully applied for the first time to investigate the reverse water-gas shift (RWGS) reaction over a 2% Pt/CeO2 catalyst. The adsorption/desorption rate constants for CO2 and H2 were determined in separate TAP pulse-response experiments, and the number of H-containing exchangeable species was determined using D2 multipulse TAP experiments. This number is similar to the amount of active sites observed in previous SSITKA experiments. The CO production in the RWGS reaction was studied in a TAP experiment using separate (sequential) and simultaneous pulsing of CO2 and H 2. A small yield of CO was observed when CO2 was pulsed alone over the reduced catalyst, whereas a much higher CO yield was observed when CO2 and H2 were pulsed consecutively. The maximum CO yield was observed when the CO2 pulse was followed by a H2 pulse with only a short (1 s) delay. Based on these findings, we conclude that an associative reaction mechanism dominates the RWGS reaction under these experimental conditions. The rate constants for several elementary steps can be determined from the TAP data. In addition, using a difference in the time scale of the separate reaction steps identified in the TAP experiments, it is possible to distinguish a number of possible reaction pathways.

Eosin Y-Functionalized Conjugated Organic Polymers for Visible-Light-Driven CO2 Reduction with H2O to CO with High Efficiency

Yu, Xiaoxiao,Yang, Zhenzhen,Qiu, Bing,Guo, Shien,Yang, Peng,Yu, Bo,Zhang, Hongye,Zhao, Yanfei,Yang, Xinzheng,Han, Buxing,Liu, Zhimin

, p. 632 - 636 (2019)

Visible-light-driven photoreduction of CO2 to energy-rich chemicals in the presence of H2O without any sacrifice reagent is of significance, but challenging. Herein, Eosin Y-functionalized porous polymers (PEosinY-N, N=1–3), with high surface areas up to 610 m2 g?1, are reported. They exhibit high activity for the photocatalytic reduction of CO2 to CO in the presence of gaseous H2O, without any photosensitizer or sacrifice reagent, and under visible-light irradiation. Especially, PEosinY-1 derived from coupling of Eosin Y with 1,4-diethynylbenzene shows the best performance for the CO2 photoreduction, affording CO as the sole carbonaceous product with a production rate of 33 μmol g?1 h?1 and a selectivity of 92 %. This work provides new insight for designing and fabricating photocatalytically active polymers with high efficiency for solar-energy conversion.

Photoelectrochemical Reduction of CO2 Coupled to Water Oxidation Using a Photocathode with a Ru(II)-Re(I) Complex Photocatalyst and a CoOx/TaON Photoanode

Sahara, Go,Kumagai, Hiromu,Maeda, Kazuhiko,Kaeffer, Nicolas,Artero, Vincent,Higashi, Masanobu,Abe, Ryu,Ishitani, Osamu

, p. 14152 - 14158 (2016)

Photoelectrochemical CO2 reduction activity of a hybrid photocathode, based on a Ru(II)-Re(I) supramolecular metal complex photocatalyst immobilized on a NiO electrode (NiO-RuRe), was confirmed in an aqueous electrolyte solution. Under half-reaction conditions, the NiO-RuRe photocathode generated CO with high selectivity, and its turnover number for CO formation reached 32 based on the amount of immobilized RuRe. A photoelectrochemical cell comprising a NiO-RuRe photocathode and a CoOx/TaON photoanode showed activity for visible-light-driven CO2 reduction using water as a reductant to generate CO and O2, with the assistance of an external electrical (0.3 V) and chemical (0.10 V) bias produced by a pH difference. This is the first example of a molecular and semiconductor photocatalyst hybrid-constructed photoelectrochemical cell for visible-light-driven CO2 reduction using water as a reductant.

Photocatalytic reduction of CO2 by CuxO nanocluster loaded SrTiO3 nanorod thin film

Shoji, Shusaku,Yin, Ge,Nishikawa, Masami,Atarashi, Daiki,Sakai, Etsuo,Miyauchi, Masahiro

, p. 309 - 314 (2016)

Photocatalytic carbon dioxide (CO2) conversion into carbon monoxide (CO) using H2O as an electron donor was achieved by the strontium titanate (SrTiO3: STO) nanorod thin films loaded with amorphous copper oxide (CuxO) nanoclusters. The loading of the CuxO-cocatalysts onto STO nanorods clearly improved the photocatalytic activity compared to bare STO nanorods. The CuxO-cocatalysts are composed of abundant and non-toxic elements, and can be loaded by using a simple and economical method. Our findings demonstrate that CuxO nanoclusters function as a general cocatalyst and can be used in combination with various semiconductors to construct low-cost and efficient photocatalytic CO2 reduction systems.

Constructing Ordered Three-Dimensional TiO2 Channels for Enhanced Visible-Light Photocatalytic Performance in CO2 Conversion Induced by Au Nanoparticles

Xue, Hairong,Wang, Tao,Gong, Hao,Guo, Hu,Fan, Xiaoli,Gao, Bin,Feng, Yaya,Meng, Xianguang,Huang, Xianli,He, Jianping

, p. 577 - 583 (2018)

As a typical photocatalyst for CO2 reduction, practical applications of TiO2 still suffer from low photocatalytic efficiency and limited visible-light absorption. Herein, a novel Au-nanoparticle (NP)-decorated ordered mesoporous TiO

Photochemical CO2 splitting by metal-to-metal charge-transfer excitation in mesoporous ZrCu(l)-MCM-41 silicate sieve

Lin, Wenyong,Frei, Heinz

, p. 1610 - 1611 (2005)

Binuclear redox sites consisting of a Zr oxo-bridged to a Cu(I) center have been obtained on the pore surface of MCM-41 silicate sieve by a stepwise grafting procedure, along with isolated metal centers. The bimetallic site features a Zr(IV)-O-Cu(I) to Zr(III)-O-Cu(II) metal-to-metal charge-transfer (MMCT) absorption extending from the UV region to about 500 nm. The Zr-O-Cu linkage is revealed by a Cu(I)-O infrared stretch mode at 643 cm-1. Irradiation of the MMCT chromophore of ZrCu(I)-MCM-41 loaded with 1 atm of CO2 gas at room temperature resulted in growth of CO (2150 cm-1) and H2O (1600 cm-1). Photolysis experiments using 13CO2 and C18O2 demonstrate that carbon monoxide and the oxygen atom of the water product originate from CO2. This indicates splitting of the CO2 by the excited MMCT moiety to CO and a surface OH radical, followed by trapping of the products at Cu(I) centers (OH is reduced to H2O). This is the first observation of CO2 photoreduction at a binuclear MMCT site at the gas-solid interface. Copyright

The main factor to improve the performance of CoSe2 for photocatalytic CO2 reduction: Element doping or phase transformation

Ding, Shujiang,Mo, Jiang,Wang, Xiaoxia,Xie, Guanqun,Xu, Yong

, p. 4457 - 4463 (2020)

In this work, orthorhombic CoSe2 is fabricated by nitrogen doping into a cubic CoSe2 structure, in which the crystalline phase undergoes transformation. The doped atoms lead to the rotation of the Se22- group, and then the faults of phase change can be observed. Thus, the reverse phase transformation provides an opportunity to study the aspects of element doping and phase change on photocatalytic CO2 reduction simultaneously. The phase change material of N-doped orthorhombic CoSe2 shows high activity toward the photoconversion of CO2 to CO, and the average production rate of CO is up to 1.66 × 104 μmol h-1 g-1 in the first 3 hours, being twice as efficient as that of cubic CoSe2. Intermediate COOH? is detected by in situ infrared spectroscopy and theoretical calculations are also conducted to reveal the intrinsic impact of the doping element on the photosplitting of CO2

A Highly Selective and Robust Co(II)-Based Homogeneous Catalyst for Reduction of CO2 to CO in CH3CN/H2O Solution Driven by Visible Light

Ouyang, Ting,Hou, Cheng,Wang, Jia-Wei,Liu, Wen-Ju,Zhong, Di-Chang,Ke, Zhuo-Feng,Lu, Tong-Bu

, p. 7307 - 7311 (2017)

Visible-light driven reduction of CO2 into chemical fuels has attracted enormous interest in the production of sustainable energy and reversal of the global warming trend. The main challenge in this field is the development of efficient, selective, and economic photocatalysts. Herein, we report a Co(II)-based homogeneous catalyst, [Co(NTB)CH3CN](ClO4)2 (1, NTB = tris(benzimidazolyl-2-methyl)amine), which shows high selectivity and stability for the catalytic reduction of CO2 to CO in a water-containing system driven by visible light, with turnover number (TON) and turnover frequency (TOF) values of 1179 and 0.032 s-1, respectively, and selectivity to CO of 97%. The high catalytic activity of 1 for photochemical CO2-to-CO conversion is supported by the results of electrochemical investigations and DFT calculations.

Enhancement of CO Evolution by Modification of Ga2O3 with Rare-Earth Elements for the Photocatalytic Conversion of CO2 by H2O

Tatsumi, Hiroyuki,Teramura, Kentaro,Huang, Zeai,Wang, Zheng,Asakura, Hiroyuki,Hosokawa, Saburo,Tanaka, Tsunehiro

, p. 13929 - 13935 (2017)

Modification of the surface of Ga2O3 with rare-earth elements enhanced the evolution of CO as a reduction product in the photocatalytic conversion of CO2 using H2O as an electron donor under UV irradiation in aqueous NaHCO3 as a pH buffer, with the rare-earth species functioning as a CO2 capture and storage material. Isotope experiments using 13CO2 as a substrate clearly revealed that CO was generated from the introduced gaseous CO2. In the presence of the NaHCO3 additive, the rare-earth (RE) species on the Ga2O3 surface are transformed into carbonate hydrates (RE2(CO3)3·nH2O) and/or hydroxycarbonates (RE2(OH)2(3-x)(CO3)x) which are decomposed upon photoirradiation. Consequently, Ag-loaded Yb-modified Ga2O3 exhibits much higher activity (209 μmol h-1 of CO) than the pristine Ag-loaded Ga2O3. The further modification of the surface of the Yb-modified Ga2O3 with Zn afforded a selectivity toward CO evolution of 80%. Thus, we successfully achieved an efficient Ag-loaded Yb- and Zn-modified Ga2O3 photocatalyst with high activity and controllable selectivity, suitable for use in artificial photosynthesis.

Efficient Photocatalytic CO2 Reduction by a Ni(II) Complex Having Pyridine Pendants through Capturing a Mg2+ Ion as a Lewis-Acid Cocatalyst

Hong, Dachao,Kawanishi, Takuya,Tsukakoshi, Yuto,Kotani, Hiroaki,Ishizuka, Tomoya,Kojima, Takahiko

, p. 20309 - 20317 (2019)

We have synthesized a new Ni(II) complex having an S2N2-tetradentate ligand with two noncoordinating pyridine pendants as binding sites of Lewis-acidic metal ions in the vicinity of the Ni center, aiming at efficient CO production in photocatalytic CO2 reduction. In the presence of Mg2+ ions, enhancement of selective CO formation was observed in photocatalytic CO2 reduction by the Ni complex with the pyridine pendants through the formation of a Mg2+-bound species, as compared to the previously reported Ni complex without the Lewis-acid capturing sites. A higher quantum yield of CO evolution for the Mg2+-bound Ni complex was determined to be 11.1percent. Even at lower CO2 concentration (5percent), the Ni complex with the pendants exhibited comparable CO production to that at the CO2-saturated concentration (100percent). The Mg2+-bound Ni complex was evidenced by mass spectrometry and 1H NMR measurements. The enhancement of CO2 reduction by the Mg2+-bound species should be derived from cooperativity between the Ni and Mg centers for the stabilization of a Ni-CO2 intermediate by a Lewis-acidic Mg2+ ion captured in the vicinity of the Ni center, as supported by DFT calculations. The detailed mechanism of photocatalytic CO2 reduction by the Ni complex with the pyridine pendants in the presence of Mg2+ ions is discussed based on spectroscopic detection of the intermediate and kinetic analysis.

Direct Z-Scheme Heterojunction of SnS2/Sulfur-Bridged Covalent Triazine Frameworks for Visible-Light-Driven CO2 Photoreduction

Guo, Shien,Yang, Peng,Zhao, Yanfei,Yu, Xiaoxiao,Wu, Yunyan,Zhang, Hongye,Yu, Bo,Han, Buxing,George, Michael W.,Liu, Zhimin

, p. 6278 - 6283 (2020)

Solar-driven reduction of CO2 into renewable carbon forms is considered as an alternative approach to address global warming and the energy crisis but suffers from low efficiency of the photocatalysts. Herein, a direct Z-Scheme SnS2/sulfur-bridged covalent triazine frameworks (S-CTFs) photocatalyst (denoted as SnS2/S-CTFs) was developed, which could efficiently adsorb CO2 owing to the CO2-philic feature of S-CTFs and promote separation of photoinduced electron–hole pairs. Under visible-light irradiation, SnS2/S-CTFs exhibited excellent performance for CO2 photoreduction, yielding CO and CH4 with evolution rates of 123.6 and 43.4 μmol g?1 h?1, respectively, much better than the most catalysts reported to date. This inorganic/organic hybrid with direct Z-Scheme structure for visible-light-driven CO2 photoreduction provides new insights for designing photocatalysts with high efficiency for solar-to-fuel conversion.

Visible-light-driven conversion of CO2 from air to CO using an ionic liquid and a conjugated polymer

Chen, Yu,Ji, Guipeng,Guo, Shien,Yu, Bo,Zhao, Yanfei,Wu, Yunyan,Zhang, Hongye,Liu, Zhenghui,Han, Buxing,Liu, Zhimin

, p. 5777 - 5781 (2017)

A metal-free and highly efficient catalytic system involving a task-specific ionic liquid, [P4444][p-2-O], and a pyrene-based conjugated polymer was developed for direct CO2 capture from air and its further photoreduction to CO under visible light irradiation, affording a CO production rate of 47.37 μmol g-1 h-1 with a selectivity of 98.3%.

Conductive Two-Dimensional Phthalocyanine-based Metal–Organic Framework Nanosheets for Efficient Electroreduction of CO2

Cao, Rong,Chai, Guo-Liang,Huang, Yuan-Biao,Si, Duan-Hui,Wu, Qiao,Xie, Ruikuan,Yi, Jun-Dong,Yin, Qi,Zhang, Meng-Di

, p. 17108 - 17114 (2021)

The electrocatalytic conversion of CO2 into value-added chemicals is a promising approach to realize a carbon-energy balance. However, low current density still limits the application of the CO2 electroreduction reaction (CO2RR). Metal–organic frameworks (MOFs) are one class of promising alternatives for the CO2RR due to their periodically arranged isolated metal active sites. However, the poor conductivity of traditional MOFs usually results in a low current density in CO2RR. We have prepared conductive two-dimensional (2D) phthalocyanine-based MOF (NiPc-NiO4) nanosheets linked by nickel-catecholate, which can be employed as highly efficient electrocatalysts for the CO2RR to CO. The obtained NiPc-NiO4 has a good conductivity and exhibited a very high selectivity of 98.4 % toward CO production and a large CO partial current density of 34.5 mA cm?2, outperforming the reported MOF catalysts. This work highlights the potential of conductive crystalline frameworks in electrocatalysis.

Direct detection of key reaction intermediates in photochemical CO 2 reduction sensitized by a rhenium bipyridine complex

Kou, Youki,Nabetani, Yu,Masui, Dai,Shimada, Tetsuya,Takagi, Shinsuke,Tachibana, Hiroshi,Inoue, Haruo

, p. 6021 - 6030 (2014)

Photochemical CO2 reduction sensitized by rhenium-bipyridyl complexes has been studied through multiple approaches during the past several decades. However, a key reaction intermediate, the CO2-coordinated Re-bipyridyl complex, which should govern the activity of CO2 reduction in the photocatalytic cycle, has never been detected in a direct way. In this study on photoreduction of CO2 catalyzed by the 4,4′-dimethyl-2,2′-bipyridine (dmbpy) complex, [Re(dmbpy)(CO) 3Cl] (1), we successfully detect the solvent-coordinated Re complex [Re(dmbpy)(CO)3DMF] (2) as the light-absorbing species to drive photoreduction of CO2. The key intermediate, the CO 2-coordinated Re-bipyridyl complex, [Re(dmbpy)(CO) 3(COOH)], is also successfully detected for the first time by means of cold-spray ionization spectrometry (CSI-MS). Mass spectra for a reaction mixture with isotopically labeled 13CO2 provide clear evidence for the incorporation of CO2 into the Re-bipyridyl complex. It is revealed that the starting chloride complex 1 was rapidly transformed into the DMF-coordinated Re complex 2 through the initial cycle of photoreduction of CO2. The observed induction period in the time profile of the CSI-MS signals can well explain the subsequent formation of the CO2- coordinated intermediate from the solvent-coordinated Re-bipyridyl complex. An FTIR study of the reaction mixture in dimethyl sulfoxide clearly shows the appearance of a signal at 1682 cm-1, which shifts to 1647 cm -1 for the 13CO2-labeled counterpart; this is assigned as the CO2-coordinated intermediate, ReII-COOH. Thus, a detailed understanding has now been obtained for the mechanism of the archetypical photochemical CO2 reduction sensitized by a Re-bipyridyl complex.

Palladium-catalyzed carbonylative α-arylation of 2-oxindoles with (Hetero)aryl bromides: Efficient and complementary approach to 3-acyl-2-oxindoles

Lian, Zhong,Friis, Stig D.,Skrydstrup, Troels

, p. 9582 - 9586 (2014)

An efficient Pd-catalyzed carbonylative α-arylation of 2-oxindoles with aryl and heteroaryl bromides for the one-step synthesis of 3-acyl-2-oxindoles has been developed. This reaction proceeds efficiently under mild conditions and is complementary to the

Ultrathin and Small-Size Graphene Oxide as an Electron Mediator for Perovskite-Based Z-Scheme System to Significantly Enhance Photocatalytic CO2 Reduction

Mu, Yan-Fei,Zhang, Wen,Dong, Guang-Xing,Su, Ke,Zhang, Min,Lu, Tong-Bu

, (2020)

The judicious design of efficient electron mediators to accelerate the interfacial charge transfer in a Z-scheme system is one of the viable strategies to improve the performance of photocatalysts for artificial photosynthesis. Herein, ultrathin and small-size graphene oxide (USGO) nanosheets are constructed and employed as the electron mediator to elaborately exploit an efficient CsPbBr3-based all-solid-state Z-scheme system in combination with α-Fe2O3 for visible-light-driven CO2 reduction with water as the electron source. CsPbBr3 and α-Fe2O3 can be closely anchored on USGO nanosheets, owing to the existence of interfacial strong chemical bonding behaviors, which can significantly accelerate the photogenerated carrier transfer between CsPbBr3 and α-Fe2O3. The resultant improved charge separation efficiency endows the Z-scheme system exhibiting a record-high electron consumption rate of 147.6 μmol g?1 h?1 for photocatalytic CO2-to-CO conversion concomitant with stoichiometric O2 from water oxidation, which is over 19 and 12 times higher than that of pristine CsPbBr3 nanocrystals and the mixture of CsPbBr3 and α-Fe2O3, respectively. This work provides a novel and effective strategy for improving the catalytic activity of halide-perovskite-based photocatalysts, promoting their practical applications in the field of artificial photosynthesis.

The Homogeneous Reduction of CO2 by [Ni(cyclam)]+: Increased Catalytic Rates with the Addition of a CO Scavenger

Froehlich, Jesse D.,Kubiak, Clifford P.

, p. 3565 - 3573 (2015)

The homogeneous electrochemical reduction of CO2 by the molecular catalyst [Ni(cyclam)]2+ is studied by electrochemistry and infrared spectroelectrochemistry. The electrochemical kinetics are probed by varying CO2 substrate and proton concentrations. Products of CO2 reduction are observed in infrared spectra obtained from spectroelectrochemical experiments. The two major species observed are a Ni(I) carbonyl, [Ni(cyclam)(CO)]+, and a Ni(II) coordinated bicarbonate, [Ni(cyclam)(CO2OH)]+. The rate-limiting step during electrocatalysis is determined to be CO loss from the deactivated species, [Ni(cyclam)(CO)]+, to produce the active catalyst, [Ni(cyclam)]+. Another macrocyclic complex, [Ni(TMC)]+, is deployed as a CO scavenger in order to inhibit the deactivation of [Ni(cyclam)]+ by CO. Addition of the CO scavenger is shown to dramatically increase the catalytic current observed for CO2 reduction. Evidence for the [Ni(TMC)]+ acting as a CO scavenger includes the observation of [Ni(TMC)(CO)]+ by IR. Density functional theory (DFT) calculations probing the optimized geometry of the [Ni(cyclam)(CO)]+ species are also presented.

A hexanuclear cobalt metal-organic framework for efficient CO2 reduction under visible light

Zhao, Jiao,Wang, Qi,Sun, Chunyi,Zheng, Tiantian,Yan, Likai,Li, Mengting,Shao, Kuizhan,Wang, Xinlong,Su, Zhongmin

, p. 12498 - 12505 (2017)

Increasing global challenges including climate warming and energy shortage have stimulated worldwide explorations for efficient materials for applications in the capture of CO2 and its conversion to chemicals. In this study, a novel pillared-layer porous metal-organic framework (Co6-MOF) with high nuclearity CoII clusters has been synthesized. This material exhibited a CO2 adsorption capacity of up to 55.24 cm3 g-1 and 38.17 cm3 g-1 at 273 K and 298 K, respectively. In a heterogeneous photocatalytic system of CO2 reduction, this material, co-operated with a ruthenium-based photosensitizer, can efficiently realize CO2 to CO conversion. Under visible-light irradiation for 3 hours, 39.36 μmol CO and 28.13 μmol H2 were obtained. This result is higher than those of most of the reported MOF materials under similar conditions and to the best of our knowledge, this is the first example of a high nuclear MOF used in CO2 reduction. The rooted reasons behind the high reactivity were studied through theoretical calculation studies. The results showed that electrons on reduced [Ru(bpy)3]Cl2·6H2O (bpy = 4,4′-bipyridine) could transfer to the Co6-MOF and the adsorbed CO2 molecule on the charged Co6-MOF could be activated more facilely. This work not only clarifies the reasons for high efficiency of the CO2 photoreduction system but also points out to us the direction for designing more effective MOF materials as photocatalysts for artificial CO2 photoreduction.

Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis

Jiang, Kun,Siahrostami, Samira,Akey, Austin J.,Li, Yanbin,Lu, Zhiyi,Lattimer, Judith,Hu, Yongfeng,Stokes, Chris,Gangishetty, Mahesh,Chen, Guangxu,Zhou, Yawei,Hill, Winfield,Cai, Wen-Bin,Bell, David,Chan, Karen,N?rskov, Jens K.,Cui, Yi,Wang, Haotian

, p. 950 - 960 (2017)

Utilizing solar energy to fix CO2 with water into chemical fuels and oxygen, a mimic process of photosynthesis in nature, is becoming increasingly important but still challenged by low selectivity and activity, especially in CO2 electrocatalytic reduction. Here, we report transition-metal atoms coordinated in a graphene shell as active centers for aqueous CO2 reduction to CO with high faradic efficiencies over 90% under significant currents up to ~60 mA/mg. We employed three-dimensional atom probe tomography to directly identify the single Ni atomic sites in graphene vacancies. Theoretical simulations suggest that compared with metallic Ni, the Ni atomic sites present different electronic structures that facilitate CO2-to-CO conversion and suppress the competing hydrogen evolution reaction dramatically. Coupled with Li+-tuned Co3O4 oxygen evolution catalyst and powered by a triple-junction solar cell, our artificial photosynthesis system achieves a peak solar-to-CO efficiency of 12.7% by using earth-abundant transition-metal electrocatalysts in a pH-equal system. Using clean electricity to reduce CO2 to chemicals or fuels is becoming increasingly important to renewable energy applications and environmental protection. The challenge comes from the strong competition with the hydrogen evolution reaction in aqueous solutions, especially for those earth-abundant transition metals such as Ni, which dramatically lowers the CO2 reduction selectivity. Isolating the transition-metal single atoms into a graphene matrix can significantly tune their catalytic behaviors to favor the CO2-to-CO reduction pathway, reaching a high CO selectivity of more than 90%. This work creates an important platform in designing active and low-cost CO2 reduction catalysts with high selectivity toward fuels, opening up great opportunities for both technological applications in renewable energies and fundamental mechanism studies in catalysis. State-of-the-art three-dimensional atom probe tomography provides direct evidence of Ni single atoms coordinated in graphene vacancies for highly selective CO2 reduction to CO and suppressed hydrogen evolution in water.

Tailored Linker Defects in UiO-67 with High Ligand-to-Metal Charge Transfer toward Efficient Photoreduction of CO2

Zhao, Xiaoxue,Xu, Mengyang,Song, Xianghai,Liu, Xin,Zhou, Weiqiang,Wang, Huiqin,Huo, Pengwei

, p. 1765 - 1777 (2022/01/27)

Defect engineering can be used as a potential tool to activate metal-organic frameworks by regulating the pore structure, electronic properties, and catalytic activity. Herein, linker defects were effectively controlled by adjusting the amount of formic acid, and UiO-67 with different CO2 reduction capabilities was obtained. Among them, UiO-67-200 had the highest ability to selectively reduce CO2 to CO (12.29 μmol g-1 h-1). On the one hand, the results based on time-resolved photoluminescence decay curves and photochemical experiments revealed that UiO-67-200 had the highest charge separation efficiency. On the other hand, the linker defects affected the band structure of UiO-67 by changing the lowest unoccupied molecular orbital (LUMO) based on the density functional theory and UV-vis spectra. Hence, the proper linker defects enhanced the ligand-to-metal charge transfer process by promoting the transfer of electrons between the highest occupied molecular orbital and LUMO. Additionally, in situ Fourier transform infrared spectra and 13CO2 labeling experiments also indicated that COOH? was an important intermediate for CO formation and that CO originated from the photoreduction of CO2.

Developing Atomically Thin Li1.81H0.19Ti2O5·2H2O Nanosheets for Selective Photocatalytic CO2Reduction to CO

Gao, Shan,Gui, Jiaojiao,Jin, Xin,Li, Yunkai,Song, Jimei,Xie, Yi,Xue, Jingyu,Yang, Chen,Yu, Yu,Zhan, Xiaowen,Zhang, Kaifu

, p. 523 - 530 (2022/01/08)

Solar-driven CO2 conversion to carbon-based fuels is an attractive approach to alleviate the worsening global climate change and increasing energy issues. However, exploring and designing efficient photocatalysts with excellent activity and stability still remain challenging. Herein, layered Li1.81H0.19Ti2O5·2H2O (LHTO) nanosheets were explored as the photocatalyst for photocatalytic CO2 reduction, and atomically thin LHTO nanosheets with one-unit-cell thickness were successfully constructed for photocatalytic CO2 reduction. The atomically thin LHTO nanosheets exhibited excellent performance for CO2 photoreduction to CO, with a yield rate of 4.0 μmol g-1 h-1, a selectivity of 93%, and over 25 h photostability, dramatically outperforming the bulk LHTO. The better performance of the atomically thin LHTO nanosheets was experimentally verified to benefit from more sites for CO2 adsorption, faster electron transfer rate, and a more negative conduction band edge compared with bulk LHTO. This work provided a methodological basis for designing more efficient photocatalytic CO2 reduction catalysts.

Insights into Transformation of Icosahedral PdRu Nanocrystals into Lattice-Expanded Nanoframes with Strain Enhancement in Electrochemical Redox Reactions

Kao, Chen-Rui,Yeh, Ai-Hsuan,Chen, Bo-Hao,Lyu, Lian-Ming,Chuang, Yu-Chun,Sneed, Brian T.,Kuo, Chun-Hong

, p. 2282 - 2291 (2022/03/01)

Bimetallic icosahedral nanoframes have three-dimensional open structures, a high surface-area-to-volume ratio, and high surface site availability. Twin boundaries in these structures cause surface lattice expansion that leads to tensile strain over the nanoframes, which can improve their catalytic activity; however, robust methods for their synthesis in most metal systems are still lacking. In this work, we demonstrate a one-step synthetic strategy for the synthesis of both closed solid and hollow frame icosahedral PdRu nanoparticles (INPs) via a two-stage process of growth and dissolution. By extraction at different reaction times, INPs, concave-faceted icosahedral PdRu nanoparticles (CINPs), and icosahedral PdRu nanoframes (INFs) are obtained. High-angle annular dark-field scanning transmission electron microscopy-energy-dispersive X-ray spectroscopy and inductively coupled plasma-optical emission spectrometry analyses show that the icosahedral nanostructures are PdRu alloys with ~5 at. % Ru relative to Pd. We also carried out the electrochemical ethanol oxidation reaction (EOR) and CO2reduction reaction over three types of catalysts, PdRu INPs, PdRu CINPs, and PdRu INFs, as well as commercial Pd NPs, to examine their catalytic properties. PdRu INFs showed a much higher mass activity than PdRu INPs, PdRu CINPs, and Pd NPs in the EOR. PdRu INFs exhibited the highest Faradaic efficiency of CO gas (34%), which suggests that the expansive strain in the framework catalyst structure improves selectivity and activity for CO2conversion.

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