Prototyping an ionization source for non-engineers

Novel mass spectrometry (MS) based analytical platforms have enabled scientists to detect and quantify molecules within biological and environmental samples more accurately. Novel MS instrumentation starts as a prototype and, after years of development, can become a commercial product to be used by the larger MS community. Without the initial prototype, many MS-based instruments today would not be produced. Additionally, biotechnology companies are the main drivers for research, development, and production of novel instruments, but the tools for prototyping instrumentation have never been more accessible. Here, we present a tutorial on prototyping instrumentation through the case study of developing the Next Generation IR-MALDESI source to show that an engineering degree is not required to design and construct a prototype instrument with modern hardware and software. We discuss the prototyping process, the necessary skills required for efficient prototyping, and information about common hardware and software used within initial prototypes.     

ChemInform Abstract: Photoelectron Spectroscopy and ab initio Study of the Structure and Bonding of Al7N‐ and Al7N.

ChemInform is a weekly Abstracting Service, delivering concise information at a glance that was extracted from about 200 leading journals. To access a ChemInform Abstract of an article which was published elsewhere, please select a “Full Text” option. The original article is trackable via the “References” option.     

Making and Breaking of C−N Bonds: Applications in the Synthesis of Unsymmetric Tertiary Amines and α-Amino Carbonyl Derivatives

An operationally simple process has been developed for the synthesis of unsymmetrical amines and α-amino carbonyl derivatives in the absence of a catalyst, ligand, oxidant, or any additives. Contrary to known reductive amination methods, this protocol is amenable to substrates containing other reducible groups. This process effectively results in consecutive cleavage and formation of C−N bonds. DFT studies and Hammett analysis provide useful insight into the mechanism. The role of noncovalent interactions as a stabilizing factor have been examined in the protocol. A wide range of alkyl-bromides have been coupled efficiently with a variety of dimethyl anilines to get unsymmetric tertiary amines with yields up to 90%. This methodology was further extended to the synthesis of α-amino carbonyl derivatives with yields up to 93%.     

A Coordination Polymer of Vaska's Complex as a Heterogeneous Catalyst for the Reductive Formation of Enamines from Amides

Low-valent metal–organic frameworks (LVMOFs) and related materials have gained interest due to their potential applications in heterogeneous catalysis. However, of the few LVMOFs that have been reported, none have shown catalytic activity. Herein, a low-valent metal-organic material constructed from phosphine linkers and Ir^I nodes is reported. This material is effectively a crystalline, insoluble analogue of Vaska's complex. As such, the material reversibly binds O₂ and catalyzes the reductive formation of enamines from amides.     

Electrode-Potential-Driven Dissociation of N-Heterocycle/BF3 Adducts: A Possible Manifestation of the Electro-Inductive Effect

Recently, non-Faradaic effects were used to modify the electronic structure and reactivity of electrode-bound species. We hypothesize that these electrostatic perturbations could influence the chemical reactivity of electrolyte species near an electrode in the absence of Faradaic electron transfer. A prime example of non-Faradaic effects is acid-base dissociation near an interface. Here, we probed the near-electrode dissociation of N-heterocycle-BF₃ Lewis adducts upon electrode polarization, well outside of the redox potential window of the adducts. Using scanning electrochemical microscopy and confocal fluorescence spectroscopy, we detected a potential-dependent depletion of the adduct near the electrode. We propose an electro-inductive effect where a more positive potential leads to electron withdrawal on the N-heterocycle. This study takes a step forward in the use of electrostatics at electrochemical interfaces for field-driven electrocatalytic and electro-synthetic processes.     

g-B3C2N3: A Potential Two Dimensional Metal-free Photocatalyst for Overall Water Splitting**

Based on hybrid density functional theory (DFT) calculations, we propose a new two-dimensional (2D) B-C-N material, graphitic- (g- ), with the promising prospect of metal-free photocatalysis. We find it to be a near ultraviolet (UV) absorbing direct band gap (3.69 eV) semiconductor with robust dynamical and mechanical stability. Estimating the band positions with respect to water oxidation and hydrogen reduction potential levels along with a detailed analysis of reaction mechanism of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), we observe that g- monolayer can be efficiently used for hydrogen fuel generation over entire pH range as well as for spontaneous water splitting at basic pH range. Upon biaxial strain application, band positions get realigned along with the free energy change that is involved in HER and OER. Consequently, operational range of pH for OER gets broadened and the proposed material exhibits the ability to perform spontaneous and simultaneous oxidation and reduction even in neutral pH. The combination of pH variation and applied strain can be used as a key to control the reducing and/or oxidizing abilities precisely for diverse photocatalytic reactions to attain environmental sustainability.     

Higher Flavor Symmetries in the Standard Model

A study of the generalized global flavor symmetries of the Standard Model is initiated. The presence of nonzero triangle diagrams between the U(3)⁵ flavor currents and the $U{(1)}_Y$ hypercharge current intertwines them in the form of a higher-group which mixes the zero-form flavor symmetries with the one-form magnetic hypercharge symmetry. This higher symmetry structure greatly restricts the possible flavor symmetries that may remain unbroken in any ultraviolet completion that includes magnetic monopoles. In the context of unification, this implies tight constraints on the combinations of fermion species which may be joined into multiplets. Three of four elementary possibilities are reflected in the classic unification models of Georgi–Glashow, $SO(10)$, and Pati–Salam. The final pattern is realized non-trivially in trinification, which exhibits the sense in which Standard Model Yukawa couplings which violate these flavor symmetries may be thought of as spurions of the higher-group. Such modifications of the ultraviolet flavor symmetries are possible only if new vector-like matter is introduced with masses suppressed from the unification scale by the Yukawa couplings.     

Organic Supercapacitors as the Next Generation Energy Storage Device: Emergence,Opportunity, and Challenges

Harnessing new materials for developing high-energy storage devices set off research in the field of organic supercapacitors. Various attractive properties like high energy density, lower device weight, excellent cycling stability, and impressive pseudocapacitive nature make organic supercapacitors suitable candidates for high-end storage device applications. This review highlights the overall progress and future of organic supercapacitors. Sustainable energy production and storage depend on low cost, large supercapacitor packs with high energy density. Organic supercapacitors with high pseudocapacitance, lightweight form factor, and higher device potential are alternatives to other energy storage devices. There are many recent ongoing research works that focus on organic electrolytes along with the material aspect of organic supercapacitors. This review summarizes the current research status and the chemistry behind the storage mechanism in organic supercapacitors to overcome the challenges and achieve superior performance for future opportunities.