keyword
https://read.qxmd.com/read/38535684/rational-design-of-a-portable-chemometric-assisted-voltammetric-sensor-based-on-ion-imprinted-polymeric-film-for-co-ii-determination-in-water
#1
JOURNAL ARTICLE
Sabrina Di Masi, Nelson Arturo Manrique Rodriguez, Marco Costa, Giuseppe Egidio De Benedetto, Cosimino Malitesta
Herein, chemometric-assisted synthesis of electrochemical sensors based on electropolymerised ion-imprinted polymeric (e-IIP) films was explored. Co(II)-IIPs sensors were prepared by performing electropolymerisation procedures of polymerisation mixtures comprising varying concentrations of an electroactive o-aminophenol (o-AP) monomer and Co(II) ions, respectively, according to the Taguchi L9 experimental design, exploiting the simultaneous evaluation of other controlled parameters during electrosynthesis. Each e-IIP developed from Taguchi runs was compared with the respective non-imprinted polymer (NIP) films and fitted according to Langmuir-Freudlich isotherms...
March 18, 2024: Nanomaterials
https://read.qxmd.com/read/38530325/highly-efficient-electrosynthesis-of-glycine-over-an-atomically-dispersed-iron-catalyst
#2
JOURNAL ARTICLE
Yingying Cheng, Shiqiang Liu, Jiapeng Jiao, Meng Zhou, Yiyong Wang, Xueqing Xing, Zhongjun Chen, Xiaofu Sun, Qinggong Zhu, Qingli Qian, Congyang Wang, Huizhen Liu, Zhimin Liu, Xinchen Kang, Buxing Han
Glycine is a nonessential amino acid that plays a vital role in various biological activities. However, the conventional synthesis of glycine requires sophisticated procedures or toxic feedstocks. Herein, we report an electrochemical pathway for glycine synthesis via the reductive coupling of oxalic acid and nitrate or nitrogen oxides over atomically dispersed Fe-N-C catalysts. A glycine selectivity of 70.7% is achieved over Fe-N-C-700 at -1.0 V versus RHE. Synergy between the FeN3 C structure and pyrrolic nitrogen in Fe-N-C-700 facilitates the reduction of oxalic acid to glyoxylic acid, which is crucial for producing glyoxylic acid oxime and glycine, and the FeN3 C structure could reduce the energy barrier of *HOOCCH2 NH2 intermediate formation thus accelerating the glyoxylic acid oxime conversion to glycine...
March 26, 2024: Journal of the American Chemical Society
https://read.qxmd.com/read/38530045/membrane-free-selective-semi-hydrogenation-of-alkynes-over-an-in-situ-formed-copper-nanoparticle-electrode
#3
JOURNAL ARTICLE
Pengyu Guo, Yousen Xu, Hao Wu, Lei Zhang
Selective semi-hydrogenation of alkynes is a significant reaction for preparing functionalized alkenes. Electrochemical semi-hydrogenation presents a sustainable alternative to the traditional thermal process. In this research, affordable copper acetylacetonate is employed as a catalyst precursor for the electrocatalytic hydrogenation of alkynes, using MeOH as the hydrogen source in an undivided cell. Good to excellent yields for both aromatic and aliphatic internal/terminal alkynes are obtained under constant current conditions...
March 26, 2024: Small
https://read.qxmd.com/read/38518115/electro-ni-dual-catalyzed-decarboxylative-c-sp3-c-sp2-cross-coupling-reactions-of-carboxylates-and-aryl-bromide
#4
JOURNAL ARTICLE
Jian Luo, Michael T Davenport, Daniel H Ess, Tianbiao Leo Liu
Paired redox-neutral electrolysis offers an attractive green platform for organic synthesis by avoiding sacrificial oxidants and reductants. Carboxylates are non-toxic, stable, inexpensive, and widely available, making them ideal nucleophiles for C-C cross-coupling reactions. Here, we report the electro/Ni dual-catalyzed redox-neutral decarboxylative C(sp3)-C(sp2) cross-coupling reactions of pristine carboxylates with aryl bromides. At a cathode, a NiII(Ar)(Br) intermediate is formed through the activation of Ar-Br bond by a NiI-bipyridine catalyst and subsequent reduction...
March 22, 2024: Angewandte Chemie
https://read.qxmd.com/read/38516798/high-performance-ammonia-electrosynthesis-from-nitrate-in-a-naoh-koh-h2o-ternary-electrolyte
#5
JOURNAL ARTICLE
Usman Bin Shahid, Yongjun Kwon, Yuan Yuan, Shuang Gu, Minhua Shao
A glut of dinitrogen-derived ammonia (NH3) over the past century has resulted in a heavily imbalanced nitrogen cycle and consequently, the large-scale accumulation of reactive nitrogen such as nitrates in our ecosystems has led to detrimental environmental issues. Electrocatalytic upcycling of waste nitrogen back into NH3 holds promise in mitigating these environmental impacts and reducing reliance on the energy-intensive Haber-Bosch process. Herein, we report a high-performance electrolyzer using an ultrahigh alkalinity electrolyte, NaOH-KOH-H2O, for low-cost NH3 electrosynthesis...
March 22, 2024: Angewandte Chemie
https://read.qxmd.com/read/38513003/validating-%C3%AE-%C3%AE-g-selectivity-descriptor-for-electrosynthesis-of-h2o2%C3%A2-from-oxygen-reduction-reaction
#6
JOURNAL ARTICLE
Dong Hyeon Mok, Seoin Back, Samira Siahrostami
Understanding selectivity trends is a crucial hurdle in the developing innovative catalysts for generating hydrogen peroxide through the two-electron oxygen reduction reaction (2e-ORR). The identification of selectivity patterns has been made more accessible through the introduction of a newly developed selectivity descriptor derived from thermodynamics, denoted as ΔΔG introduced in Chem Catal.2023, 3 (3), 100568. To validate the suitability of this parameter as a descriptor for 2e-ORR selectivity, we utilize an extensive library of 155 binary alloys...
March 21, 2024: Angewandte Chemie
https://read.qxmd.com/read/38512110/boosting-electrocatalytic-ethylene-epoxidation-by-single-atom-modulation
#7
JOURNAL ARTICLE
Hanyu Wang, Shuo Wang, Yanpeng Song, Yang Zhao, Zhenyu Li, Yuxiang Shen, Zhangquan Peng, Dunfeng Gao, Guoxiong Wang, Xinhe Bao
The electrochemical synthesis of ethylene oxide (EO) using ethylene and water under ambient conditions presents a low-carbon alternative to existing industrial production process. Yet, the electrocatalytic ethylene epoxidation route is currently hindered by largely insufficient activity, EO selectivity, and long-term stability. Here we report a single atom Ru-doped hollandite structure KIr4O8 (KIrRuO) nanowire catalyst for efficient EO production via a chloride-mediated ethylene epoxidation process. The KIrRuO catalyst exhibits an EO partial current density up to 0...
March 21, 2024: Angewandte Chemie
https://read.qxmd.com/read/38511578/artificial-and-biosynthetic-nanoparticles-boost-bioelectrochemical-reactions-via-efficient-bidirectional-electron-transfer-of-shewanella-loihica
#8
JOURNAL ARTICLE
Han Chen, Yu-Qing Wei, Meng-Yuan Xu, Ma-Wei Zhu, Junying Liu, Yang-Chun Yong, Zhen Fang
Bioelectrochemical reactions using whole-cell biocatalysts are promising carbon-neutral approaches because of their easy operation, low cost, and sustainability. Bidirectional (outward or inward) electron transfer via exoelectrogens plays the main role in driving bioelectrochemical reactions. However, the low electron transfer efficiency seriously inhibits bioelectrochemical reaction kinetics. Here, a three dimensional and artificial nanoparticles-constituent inverse opal-indium tin oxide (IO-ITO) electrode is fabricated and employed to connect with exoelectrogens (Shewanella loihica PV-4)...
March 21, 2024: Small
https://read.qxmd.com/read/38511543/anchoring-ultrafine-%C3%AE-mo-2-c-clusters-inside-porous-co-nc-using-mofs-for-electric-powered-coproduction-of-valuable-chemicals
#9
JOURNAL ARTICLE
Yu-Zhen Chen, Yi-Wen Fan, Yang Wang, Zhibo Li
Electroredox of organics provides a promising and green approach to producing value-added chemicals. However, it remains a grand challenge to achieve high selectivity of desired products simultaneously at two electrodes, especially for non-isoelectronic transfer reactions. Here a porous heterostructure of Mo2 C@Co-NC is successfully fabricated, where subnanometre β-Mo2 C clusters (<1 nm, ≈10 wt%) are confined inside porous Co, N-doped carbon using metalorganic frameworks. It is found that Co species not only promote the formation of β-Mo2 C but also can prevent it from oxidation by constructing the heterojunctions...
March 21, 2024: Small
https://read.qxmd.com/read/38507716/enhancing-h-2-o-2-electrosynthesis-at-industrial-relevant-current-in-acidic-media-on-diatomic-cobalt-sites
#10
JOURNAL ARTICLE
Helai Huang, Mingze Sun, Shuwei Li, Shengbo Zhang, Yiyang Lee, Zhengwen Li, Jinjie Fang, Chengjin Chen, Yu-Xiao Zhang, Yanfen Wu, Yizhen Che, Shuairen Qian, Wei Zhu, Cheng Tang, Zhongbin Zhuang, Liang Zhang, Zhiqiang Niu
Electrocatalytic synthesis of hydrogen peroxide (H2 O2 ) in acidic media is an efficient and eco-friendly approach to produce inherently stable H2 O2 , but limited by the lack of selective and stable catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction to efficiently produce H2 O2 at 50-400 mA cm-2 in acid. Electrode kinetics study shows a >95% selectivity for two-electron oxygen reduction on the diatomic cobalt sites. In a flow cell device, a record-high production rate of 11...
March 20, 2024: Journal of the American Chemical Society
https://read.qxmd.com/read/38503346/long-term-continuous-ammonia-electrosynthesis
#11
JOURNAL ARTICLE
Shaofeng Li, Yuanyuan Zhou, Xianbiao Fu, Jakob B Pedersen, Mattia Saccoccio, Suzanne Z Andersen, Kasper Enemark-Rasmussen, Paul J Kempen, Christian Danvad Damsgaard, Aoni Xu, Rokas Sažinas, Jon Bjarke Valbæk Mygind, Niklas H Deissler, Jakob Kibsgaard, Peter C K Vesborg, Jens K Nørskov, Ib Chorkendorff
Ammonia is crucial in fertilizer and chemical industries and is seen as a carbon-free fuel1 . The ammonia electrosynthesis from nitrogen at ambient conditions offers an attractive alternative to the Haber-Bosch process2,3 . The lithium-mediated nitrogen reduction (Li-NRR) represents a promising approach for continuous-flow ammonia electrosynthesis, coupling nitrogen reduction with hydrogen oxidation4 . However, tetrahydrofuran (THF), commonly used as a solvent, impedes long-term ammonia production due to polymerization and volatility issues...
March 19, 2024: Nature
https://read.qxmd.com/read/38499554/phenol-as-proton-shuttle-and-buffer-for-lithium-mediated-ammonia-electrosynthesis
#12
JOURNAL ARTICLE
Xianbiao Fu, Aoni Xu, Jakob B Pedersen, Shaofeng Li, Rokas Sažinas, Yuanyuan Zhou, Suzanne Z Andersen, Mattia Saccoccio, Niklas H Deissler, Jon Bjarke Valbæk Mygind, Jakob Kibsgaard, Peter C K Vesborg, Jens K Nørskov, Ib Chorkendorff
Ammonia is a crucial component in the production of fertilizers and various nitrogen-based compounds. Now, the lithium-mediated nitrogen reduction reaction (Li-NRR) has emerged as a promising approach for ammonia synthesis at ambient conditions. The proton shuttle plays a critical role in the proton transfer process during Li-NRR. However, the structure-activity relationship and design principles for effective proton shuttles have not yet been established in practical Li-NRR systems. Here, we propose a general procedure for verifying a true proton shuttle and established design principles for effective proton shuttles...
March 18, 2024: Nature Communications
https://read.qxmd.com/read/38497122/highly-coordinative-molecular-cobalt-phthalocyanine-electrocatalyst-on-an-oxidized-single-walled-carbon-nanotube-for-efficient-hydrogen-peroxide-production
#13
JOURNAL ARTICLE
Yaoxin Li, Haoying Cheng, Meilin Wang, Jiaoxing Xu, Lunhui Guan
H2 O2 production via the two-electron oxygen reduction reaction (2e- ORR) offers a potential alternative to the current anthraquinone method owing to its efficiency and environmental friendliness. However, it is necessary to determine the structures of electrocatalysts with cost-effectiveness and high efficiency for future industrialization demand. Herein, a supramolecular catalyst composed of cobalt-phthalocyanine on a near-monodispersed and oxidized single-walled carbon nanotube (CoPc/o-SWCNT) was synthesized via a solution self-assembly method for catalyzing the 2e- ORR for H2 O2 electrosynthesis...
March 18, 2024: Materials Horizons
https://read.qxmd.com/read/38496047/the-nexus-of-innovation-electrochemically-synthesizing-h-2-o-2-and-its-integration-with-downstream-reactions
#14
REVIEW
Qiu Jiang, Yuan Ji, Tingting Zheng, Xu Li, Chuan Xia
Hydrogen peroxide (H2 O2 ) represents a chemically significant oxidant that is prized for its diverse applicability across various industrial domains. Recent innovations have shed light on the electrosynthesis of H2 O2 through two-electron oxygen reduction reactions (2e- ORR) or two-electron water oxidation reactions (2e- WOR), processes that underscore the attractive possibility for the on-site production of this indispensable oxidizing agent. However, the translation of these methods into practical utilization within chemical manufacturing industries remains an aspiration rather than a realized goal...
March 13, 2024: ACS Mater Au
https://read.qxmd.com/read/38477685/a-wetting-and-capture-strategy-overcoming-electrostatic-repulsion-for-electroreduction-of-nitrate-to-ammonia-from-low-concentration-sewage
#15
JOURNAL ARTICLE
Yinghao Xue, Qihui Yu, Junhua Fang, Yan Jia, Rongchang Wang, Jianwei Fan
Ammonia production by electrocatalytic nitrate reduction reaction (NO3 RR) in water streams is anticipated as a zero-carbon route. Limited by dilute nitrate in natural sewage and the electrostatic repulsion between NO3 - and cathode, NO3 RR can hardly be achieved energy-efficiently. The hydrophilic Cu@CuCoO2 nano-island dispersed on support can enrich NO3 - and produce a sensitive current response, followed by electrosynthesis of ammonia through atomic hydrogen (*H) is reported. The accumulated NO3 - can be partially converted to NO2 - without external electric field input, confirming that the Cu@CuCoO2 nano-island can strongly bind NO3 - and then trigger the reduction via dynamic evolution between Cu-Co redox sites...
March 13, 2024: Small
https://read.qxmd.com/read/38470826/selective-electrified-propylene-to-propylene-glycol-oxidation-on-activated-rh-doped-pd
#16
JOURNAL ARTICLE
Jianan Erick Huang, Yiqing Chen, Pengfei Ou, Xueda Ding, Yu Yan, Roham Dorakhan, Yanwei Lum, Xiao-Yan Li, Yang Bai, Chengqian Wu, Mengyang Fan, Mi Gyoung Lee, Rui Kai Miao, Yanjiang Liu, Colin O'Brien, Jinqiang Zhang, Cong Tian, Yongxiang Liang, Yi Xu, Mingchuan Luo, David Sinton, Edward H Sargent
Renewable-energy-powered electrosynthesis has the potential to contribute to decarbonizing the production of propylene glycol, a chemical that is used currently in the manufacture of polyesters and antifreeze and has a high carbon intensity. Unfortunately, to date, the electrooxidation of propylene under ambient conditions has suffered from a wide product distribution, leading to a low faradic efficiency toward the desired propylene glycol. We undertook mechanistic investigations and found that the reconstruction of Pd to PdO occurs, followed by hydroxide formation under anodic bias...
March 12, 2024: Journal of the American Chemical Society
https://read.qxmd.com/read/38470010/accelerated-dynamic-reconstruction-in-metal-organic-frameworks-with-ligand-defects-for-selective-electrooxidation-of-amines-to-azos-coupling-with-hydrogen-production
#17
JOURNAL ARTICLE
Lingzhi Sun, Xun Pan, Ya-Nan Xie, Jingui Zheng, Shaohan Xu, Lina Li, Guohua Zhao
Electrosynthesis coupled hydrogen production (ESHP) mostly involves catalyst reconstruction in aqueous phase, but accurately identifying and controlling the process is still a challenge. Herein, we modulated the electronic structure and exposed unsaturated sites of metal-organic frameworks (MOFs) via ligand defect to promote the reconstruction of catalyst for azo electrosynthesis (ESA) coupled with hydrogen production overall reaction. The monolayer Ni-MOFs achieved 89.8% Faraday efficiency and 90.8% selectivity for the electrooxidation of 1-methyl-1H-pyrazol-3-amine (Pyr-NH2) to azo, and an 18...
March 12, 2024: Angewandte Chemie
https://read.qxmd.com/read/38466222/mechanistic-insights-into-surfactant-modulated-electrode-electrolyte-interface-for-steering-h-2-o-2-electrosynthesis
#18
JOURNAL ARTICLE
Yu Fan, Yuxin Chen, Wangxin Ge, Lei Dong, Yanbin Qi, Cheng Lian, Xiaodong Zhou, Honglai Liu, Zhen Liu, Hongliang Jiang, Chunzhong Li
Electrocatalytic reactions taking place at the electrified electrode-electrolyte interface involve processes of proton-coupled electron transfer. Interfacial protons are delivered to the electrode surface via a H2 O-dominated hydrogen-bond network. Less efforts are made to regulate the interfacial proton transfer from the perspective of interfacial hydrogen-bond network. Here, we present quaternary ammonium salt cationic surfactants as electrolyte additives for enhancing the H2 O2 selectivity of the oxygen reduction reaction (ORR)...
March 11, 2024: Journal of the American Chemical Society
https://read.qxmd.com/read/38456779/electrosynthesis-of-h-2-o-2-promoted-by-%C3%AF-%C3%AF-interaction-on-a-metal-free-carbon-catalyst
#19
JOURNAL ARTICLE
Jiating Qu, Guifa Long, Lin Luo, Yang Yang, Wenjun Fan, Fuxiang Zhang
The synthesis of hydrogen peroxide (H2 O2 ) through electrocatalytic oxygen reduction reaction is an ideal alternative to the current energy-intensive anthraquinone process, but developing cost-effective and high-efficiency electrocatalysts is still challenging. Herein, a metal-free graphitic carbon nitride/carbon nanotube (g-C3 N4 /CNT) hybrid catalyst can enhance H2 O2 production via π-π interaction is reported, achieving almost unity (97%) H2 O2 production at 0.57 V with high selectivity of over 92% across the wide potential range from 0...
March 8, 2024: Small
https://read.qxmd.com/read/38456336/utilisation-of-carbon-dioxide-and-nitrate-for-urea-electrosynthesis-with-a-cu-based-metal-organic-framework
#20
JOURNAL ARTICLE
Meng-Di Zhang, Jia-Run Huang, Pei-Qin Liao, Xiao-Ming Chen
It is important and challenging to utilise CO2 and NO3 - as a feedstock for electrosynthesis of urea. Herein, we reported a stable 2D metal-organic framework (MOF) Cu-HATNA, possessing planar CuO4 active sites, as an efficient electrocatalyst for coupling CO2 and NO3 - into urea, achieving a high yield rate of 1.46 g h-1 gcat -1 with a current density of 44.2 mA cm-1 at -0.6 V vs. RHE. This performance surpasses most of the previously reported catalysts, revealing the great prospects of MOFs in sustainable urea synthesis...
March 8, 2024: Chemical Communications: Chem Comm
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